The 28-year-old, who has played nearly 200 games for the London side since joining them in 2006, takes over as skipper from England prop Joe Marler.
"Since I moved to Quins nine years ago it has felt like home to me and I want to repay that by doing the captaincy role justice, like so many other great captains who have done the job before me," Care told the club website.
"It will be great to have the experience of other leaders like Chris (Robshaw), Joe (Marler), Nick Easter and Nick Evans as well as Mike (Brown) around me, who have all been at the club for so long," Care, who is in England's World Cup squad, added.
"I know they will make my job a lot easier and support me in the role both on and off the field."
Harlequins director of rugby Conor O'Shea believes Care's attacking style epitomised the way he likes his team to play.
"In making Danny captain we are making a statement as to how we intend to play and challenge for the title again," O'Shea said.
"I have watched Danny grow from a boy to a man, learning lessons along the way and he is now ready to take all that learning and apply it in a leadership role."
Marler took over as Harlequins captain last year from England skipper Robshaw.
(Reporting by Ed Osmond; editing by Sudipto Ganguly)
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