Carroll joins Olympiakos from OFI Crete and has signed an 18-month contract with the club.
“I’m very happy to have joined such a club,” he told the club’s official website.
“It’s a real honour to be part of Olympiakos, Greece’s greatest team. I will do my best in order to contribute and help our squad accomplish its goals.
“I’m really looking forward to the Europa League games and my own comeback to European competition.
“I’m hoping that next year we will be playing in the Champions League, because everybody wants to play at the top level. In order to be able to do so, however, we must first win the championship.”