"I'm coming to you and into the club which is mine now... I want to win together," the 42-year-old said in a brief video message to the club's fans.
The league got off to a rousing start last year with Brazilian Zico headlining the managers' list while marquee players included Italian duo Alessandro Del Piero and Marco Materazzi, and Frenchman Nicholas Anelka.
Zico has returned for his second year at the helm of FC Goa, who also signed Carlos' 2002 World Cup-winning teammate and former Bayern Munich defender Lucio as their marquee player.
Anelka also returned to Mumbai City FC, this time as player-cum-coach.
Carlos, famous for his free-kick prowess during his playing days, replaces Dutchman Harm van Veldhoven, under whom Delhi finished at fifth spot last year.
The second season of the eight-team league, boasting of celebrity owners, kicks off on Oct. 3.
(Reporting by Amlan Chakraborty in New Delhi; editing by Sudipto Ganguly)
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