According to The Hollywood Reporter, Andy and Lana Wachowski have sold the script Hood - a modern-day "urban" take on the Nottingham outlaw - to Warner Bros and will direct the project with Smith as a potential leading man.
Smith famously turned down the chance to play Neo in the duo's sci-fi hit The Matrix, but has insisted that he doesn't regret the move because of the success it brought Keanu Reeves.
Errol Flynn, Sean Connery, Kevin Costner and Russell Crowe are among the stars who have previously portrayed Robin Hood on screen.
The Wachowskis' next movie, CN-9, takes place in the near future and flashes back to a story about a gay relationship between a US soldier and an Iraqi during the conflict.
Arianna Huffington, Salman Rushdie, Jesse Ventura and Cornel West have reportedly filmed talking head scenes for the secretive project.