PTI said Devsaab, who millions of his fans felt would live forever, died of a heart attack.
He was 89.
The last rites will be conducted in London.
Dev Anand won two Filmfare Awards -- in 1958 for Kala Paani and in 1966 for Guide.
Guide won Filmfare Awards in five other categories including Best Film and Best Director and was India's entry for the Oscars in the foreign film category that year.
In 1993, he received a Filmfare Lifetime Achievement Award and in 1996 he received a Screen Videocon Lifetime Achievement Award.
Devsaab was involved with a new project Song Of Life -- he was to play the central character -- when he died.
Devsaab's late brothers Chetan Anand and Vijay Anand were also movie directors. Their sister Sheel Kanta Kapur is director Shekhar Kapur's mother.
Please listen to Dev Anand's best songs here
Also see: Dev Anand on the Rediff Chat
There is no business like show business: Dev Anand
Bollywood's man for all seasons
Dev Anand's best movies
The women in Dev Anand's life
Down Memory Lane with Dev Anand
Please post your tributes to Devsaab here.
There is no business like show business says Dev Anand
Bollywood's man for all seasons
Dev Anand's best movies
The women in Dev Anand's life
Down Memory Lane with Dev Anand