The 37-year-old signed a new contract last week to take him into his 19th season at the club next year.
However, prop Will Collier confirmed this week that he is heading to the Top 14, while Andre Esterhuizen is off home to South Africa and Louis Lynagh is joining Benetton.
Collier, 33, joined Quins in 2009 and made 240 appearances winning two Premiership titles and played twice for England.
Care, who has been at the south west London club since his move from Leeds Tykes in 2006, said: "Will is one of the best blokes I've come across in the sport. A proper Harlequins legend, he's played at the club for such a long time after supporting us as a child.
"It's a massive move for him and his family, we would have loved to have reached a European final with him but it wasn't meant to be.
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