Harlequins
At the end of the 2005–06 season Care left Leeds Tykes and signed a 3 year contract with Harlequins. Before joining his new club he was a member of the England squad taking part in the IRB Under-21 World Championship in France, making his debut at that level in the opening game against Fiji which England won 34–8. He won 4 caps during the tournament including a starting appearance in the 5th/6th place game against Ireland. Care scored the first try in England's 32–8 victory which gave them 5th place, their highest ever finishing position in the competition.
At Harlequins Care initially found himself understudying Samoan international Steve So'oialo at scrum-half but after disappointing results early in the season the club recruited the experienced Andy Gomarsall, a member of England's World Cup winning squad in 2003. This pushed Care down the pecking order at Harlequins and restricted his game time although he did get opportunities to start in EDF Energy Cup and European Challenge Cup games before making his first Guinness Premiership start for his new club in a memorable 9–3 home win against Bath in January 2007. Later that month he was named as captain of the England Under-20 team for the forthcoming series of Six Nations games, his first experience of captaincy at any level of the game.
Care's debut as captain saw England gain a comfortable 31–5 victory over Scotland at Bath although he was forced to leave the field early in the second half with a bruised hip. A week later Care had recovered sufficiently from his injury to lead his side to a 30–10 victory over Italy, again at Bath, with Care contributing a drop goal in the second half. However England's Grand Slam ambitions were thwarted in the next game 2 weeks later when they lost narrowly 13–6 against Ireland in Athlone. England finished the championship in 3rd place after losing 32–13 to France at Northampton and drawing 21–21 against Wales at Newport with Care captaining the side in all 5 games.
After completing the Six Nations Championship with the England Under-20 team Care was recalled to the England Sevens squad for the Hong Kong and Adelaide legs of the IRB Sevens Tournament during late March / early April 2007. England were knocked out at the quarter final stage in both tournaments. In Hong Kong they lost to New Zealand and in Adelaide they were beaten by Kenya.
At the end of the season Care was part of the Harlequins squad which won the London Floodlit Sevens title at Rosslyn Park for the first time since 1987 before joining up again with the England Sevens squad for the final legs of the 2006/2007 IRB Sevens series at Twickenham and Murrayfield. At Twickenham England failed to qualify for the quarter finals of the Cup after a disastrous 22–0 defeat at the hands of Wales on Day 1. The highlight for Care was a hat-trick of tries in a 17–14 victory over South Africa. On Day 2 England beat Kenya, France and Portugal to win the Bowl competition.
A week later at Murrayfield England again disappointed on Day 1 by failing to qualify for the quarter finals of the Cup after defeats against Argentina and New Zealand. However, once again the team bounced back strongly on Day 2 to win the Bowl beating Portugal 31–0 in the final. Due to the late withdrawal from the squad of England Sevens captain Simon Amor following the birth of his first child, Care was asked to take on additional responsibility by assuming the main play-maker role within the team. He responded by being the 2nd highest scorer in the tournament with 42 points (4 tries + 11 conversions) including 2 spectacular individual tries in a thrilling 24–19 victory over Australia in the Bowl semi-final which went into extra-time.
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