Smith, 37, who is currently visiting India, said he had great regard for Indian cinema and suggested there needed to be more give and take between the film industries of India and the US.
The star of "Men In Black" and "Hitch" said: "I really feel like there is a marriage to be made between the three-act structure of American cinema and the beauty of the colour and depth of story and characters in Indian cinema.
"The most important thing is for myself to make an artistic connection with producers, directors and actors."
Smith, whose next film "Pursuit of Happiness" will be released later this year, was talking to reporters at the launch of Pix, Sony TV's new movie channel.
However, Smith ruled out any immediate joint projects with Bollywood even as he called for closer ties between Hollywood and Bollywood.
He said the US audiences would turn away from highly produced blockbuster movies in favour of the "depth of story" that, he felt, featured in Indian films.
Smith said the first Indian movie he watched was Ram Gopal Varma's "Sarkar" that starred Amitabh Bachchan - a film based on the Francis Ford Coppola classic "Godfather".
"I was really just blown away by 'Big B'. From today forward I am going to be known as the 'Big W'," Smith uipped.
He also gushed that he was a fan of Bollywood diva Aishwarya Rai, a former miss world.
"She has a powerful energy. She doesn't have to say anything, she doesn't have to do anything. Whatever she wants to make, I'm there."
India is the world's biggest producer of movies in numbers but accounts for only one percent of global film revenues.