The King's Speech director Tom Hooper is behind the project, which is based on the musical take on Victor Hugo's classic novel.
Australian actor Crowe has signed on to play Javert, the police inspector who pursues Hugh's ex-con, Jean Valjean.
Russell, 47, and Jackman, 42, will both sing in the flick.
According to US website Gossip Cop, producer Cameron Mackintosh, who originally brought the story to the stage and is now taking it to the screen, said: 'Even though I have dreamt about making the film of Les Miserables for over 25 years, I could never have imagined that we would end up with the dream director Tom Hooper, and the dream cast of Hugh Jackman and Russell Crowe as the two great protagonists Jean Valjean and Javert.'
The musical tells story of a man who steals bread to feed his sister during the 19th century French rebellion and then spends years in prison.
Les Miserables is scheduled to be released in December 2012.