The 53-year-old is best known for his turn in the James Bond film "Casino Royale". He also uses the name Gautam Paul Bhattacharjee and is a popular stage and television actor in Britain.
He was last seen at London's Royal Court Theatre on July 10 and sent a text message to his girlfriend at 9pm that night, but no one has heard from him since.
"This is totally out of character for Mr Bhattacharjee, who has appeared in numerous television and stage productions as well as films, most recently in 'Dirty Pretty Things', 'Casino Royale' and 'The Best Exotic Marigold Hotel'," Metropolitan police said in their appeal.
Bhattacharjee was captured on CCTV footage walking from the stage door area of the theatre up an external alleyway. He turned left as if "walking towards Sloane Square tube station", it said.
He was in the Royal Court's company of 14 actors performing in the weekly rep series, which sees six plays staged in six weeks. He had already appeared in two plays, including "The President Has Come to See You", in which he played the president of Georgia who is on the run and hiding in his citizens' homes.
"He left last Wednesday in good spirits but didn't make it to rehearsals the next day," a spokesperson for the theatre said.
Bhattacharjee played a doctor in "Casino Royale" (2006) and his TV work includes popular British soaps like "EastEnders" and "The Bill".
He lived between India and Britain during his childhood and is now based in Redbridge, northeast London.
TV star Stephen Fry joined hundreds of people on Twitter to express concern over Bhattacherjee's whereabouts.
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