- Dr. Diaper - A villain whose plan was to blow up the moon with the Lasermatic 2000: all the big chunks of it would come crashing down on every major city in the world. This chaos would allow him to take over the earth. He made a brief appearance at the end of the fourth book, where he met Professor Poopypants in jail and, along with all the other inmates, laughed at his name, much to Poopypants' annoyance and anger. When Poopypants, now called Tippy Tinkletrousers, alters history, Dr. Diaper succeeds in blowing up the moon, but is eaten by the Talking Toilets. This was reversed when Tippy restored history to the way it was. He was the main villain of the first book.
- Dr. Diaper's Evil Robots - They were robots created by Dr. Diaper, and assigned to steal a diamond, the power source to Dr. Diaper's Lasermatic 2000 and kidnapped Mr. Krupp (who was hypnotized to think he was Captain Underpants). They were destroyed by George and Harold. They were the secondary villains in the first book.
- The Turbo-Toilet 2000 - A giant toilet created by George and Harold, who was accidentally brought into the real world with a modified photocopier. His plan was to devour Captain Underpants and conquer the world with his army of vicious Talking Toilets, but he was defeated and flown to Uranus; in the fourth book, in the newspaper Professor Poopypants was holding, one of the articles states that there were talking toilets found on Uranus and the "Piqua Order Of Professional Space Interplanetary Explorers" (POOPSIE) later discovered the talking toilets on Uranus yet again In Book 7. It is also a running gag in the book series that bad guys get sent to Uranus. He was the main villain of the second book and will return in the eleventh book.
- The Talking Toilets - Ferocious sharp-fanged toilets who worked for the Turbo Toilet 2000. They ate all the teachers in the school, but after being fed food from the school cafeteria they vomited the unconscious-but-unharmed teachers before dying. When Tippy Tinkletrousers alters history, they take over the world and eat Dr. Diaper before they are killed presumably by the zombie nerds. However history's original events were later restored. They are the secondary villains of the second book.
- Zorx, Klax and Jennifer - Three space aliens who had the head of a frog, the face of a snake, the tentacles of an octopus and the legless body of a slug who planned to create an army of gargantuan zombies from the school's students and teachers to take over the world. They were later blown up in a horrific UFO explosion. In the alternate dimension, they are firemen with Professor Poopypants. When Tippy Tinkletrousers alters history, they are presumably spared from their fate as they are shown to have grown the zombie nerds to incredible size, but Tippy would later restore history to the way it was. They were the main villains of the third book.
- The Dandelion Of Doom - A Dandelion that drank alien rapid-growth juice, causing it to grow into a giant, evil monster. Because Captain Underpants had to drink alien superpower juice in order to defeat it, it could be considered responsible for giving Captain Underpants his superpowers. It is the secondary villain of the book.
- The Lunchroom Zombie Nerds of the Zombi Juice - After being fed the lunches, zombie nerd milkshakes served by Zorx, Klax and Jennifer the students and teachers transformed into mindless, dangerous zombie nerds. The aliens intended to use rapid-growth juice to make the zombies grow to a gigantic size, allowing the aliens to use them to conquer the world. After the aliens' defeat, George and harold returned the zombie nerds to normal by anti-zombie-nerd root beer. When Tippy Tinkletrousers alters history, they are shown to currently be in control of the world, grown to gigantic size. This is reversed when Tippy restores history. They were the tertiary villains of the third book.
- Professor Pippy Pee-Pee Poopypants (a/k/a Tippy Tinkletrousers) - A brilliant scientist who unfortunately comes from a foreign culture in which everyone has a silly name. Because of his name he was never taken seriously by any of the American universities, so he decided to go into teaching science at the school after Mr. Fyde quit - however he was eventually driven insane by being constantly made fun of and his plan was to give everyone on the planet a silly name. He was defeated by a giant Captain Underpants and was taken to jail. George and Harold convince him to change his name but it is still silly. In the alternate dimension, he is a fireman with the space aliens. The main villain of the fourth book. He reappears in the ninth book for revenge after thinking that it is George and Harold's fault that people still laugh at his name. He goes back in time to when George and Harold were in kindergarten and inadvertently causes Mr. Krupp to be fired, resulting in history being altered so Captain Underpants never existed and the world was destroyed by Dr. Diaper, the Talking Toilets, and the Zombie Nerds. Before he could undo what he did, Tippy was seemingly killed when Harold (now a giant Zombie Nerd) stomped on him, however, this turned out to be a trick due to Zombie Nerds being slow and Tippy faking his death with a pack of ketchup. He then went back in time in the tenth book and stopped himself from altering history, then shrank his younger self before battling George, Harold, and Mr. Krupp on a time traveling trip during which "Tiny Tippy" time traveled back in time a bit so that three Tippys existed at once: Big Tippy, Tiny Tippy, and Slightly Younger Tiny Tippy. Big Tippy blew himself up in a nuclear explosion that also killed the dinosaurs, Tiny Tippy used his Goosy-Grow 4000 to become Supa Mega Tippy only to be accidentally frozen in a magnified freeze beam that caused the Ice Age; and Slightly Younger Tiny Tippy grew to incredible size and blew himself up with a nuclear bomb, which, once Crackers and Sulu sent him back in time 13.7 billion years was the Big Bang (or Big Ka-Bloosh) that created the universe.
- Wedgie Woman - A villain originally created by George and Harold who was based on their teacher, Ms. Ribble. After a second mishap with the 3D Hypno-Ring the real Ms. Ribble becomes convinced that she really is Wedgie Woman - at first she has no superpowers, but after her hairstyle gets splattered with the superpower juice from the third book her hair transforms into arms and she gains super-intelligence. She is later changed back to normal by George and Harold, where she becomes nice and bakes chocolate chip cookies everyday for the class. She is the main villain of the fifth book.
- Robo-George and The Harold 2000 - Two giant robots built by Wedgie Woman based on George and Harold. They were totally obedient to Wedgie Woman, each had a vast arsenal of powerful weapons and gadgets and were programmed to destroy Captain Underpants once they heard him say "Tra-la-laaa!" They were completely destroyed by Captain Underpants when he used the Harold 2000's own hands against them. They are the secondary villains of the fifth book.
- The Bionic Booger Boy (Melvin Sneedly) - A mix of Melvin Sneedly, snot and a robot in an invention test. He went crazy after an idiotic, fat person named Mr. Snoddy threw tissues at him, the thing he hates the most. He grew bigger and more annoyed, and plotted to get revenge. He is later broken down by Sulu, George, Harold, and Mr. Sneedly, but in the process Melvin and Mr. Krupp switched bodies. He is the main villain of the sixth book.
- Carl, Trixie and Frankenbooger (The Tree Robo-Boogers) - Boogers that planned to destroy Captain Underpants. They all came from the Bionic Booger Boy. They all share a weakness to oranges, which Captain Underpants successfully used to destroy the rampaging trio of living mucus. Carl had the Bionic Booger Boy's legs, Trixie had the tentacles, and Frankenbooger had the arms. Whenever they eat, they become bigger and more evil. They are the main villains of the seventh book.
- Captain Blunderpants - The opposite of Captain Underpants from an alternate dimension who plots on taking over the world and destroying Captain Underpants. Captain Blunderpants has a toupee and looks and acts more like Mr. Krupp, while the alternate Mr. Krupp is nice. He was defeated by Boxer Boy and Great-Granny Girdle. Also his transformation is opposite; when water is splashed on him, he becomes the evil Captain Blunderpants and when someone snaps their fingers, he becomes nice Mr. Krupp.
- Evil George and Evil Harold - Evil versions of George and Harold from an alternate dimension who are both intelligent and evil. They helped Captain Blunderpants and unlike the sketchy, amateurish George and Harold they are actually good authors and illustrators (ironically the main George and Harold consider the alternative George and Harold's work inferior). Additionally, they also tended to correct the spelling on signs (while their counterparts often change the signs into funny words). They were shrunk and sent back to their universe by George and Harold.
- Kipper Krupp - A sixth-grade bully and Mr. Krupp's nephew who would bully George and Harold when they were in kindergarten. He appears in "Captain Underpants and the Terrifying Re-Turn of Tippy Tinkletrousers". After George and Harold make him think he is being haunted by a ghost, he changes his ways. When Tippy Tinkletrousers alters history by traveling to this scene with a robot resembling the ghost, Kipper and his friends go insane and are sent to Piqua Valley Home for the Reality Challenged. Mr. Krupp is blamed and is fired, resulting in the destruction of Earth, but all this is reversed when Tippy of the future goes back in time and freezes them so they never see the Robo-Pants and lose their minds, thus restoring history.
- The Bullies (Finkstien, Bugg and Loogie) are Kipper's friends and also bully George and Harold.
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Famous quotes containing the word villains:
“Why do villains have so much influence? Because the honest people are terribly dense.”
—Franz Grillparzer (17911872)
“I dont believe in villains or heroes, only in right or wrong ways that individuals are taken, not by choice, but by necessity or by certain still uncomprehended influences in themselves, their circumstances and their antecedents.”
—Tennessee Williams (19141983)