The film--only the second to be made by New Zealand-born writer-director Andrew Dominik--reminds us that Dominik's debut film, Chopper (2000), was the cunningly off-kilter portrait of another real-life criminal psychopath who became a kind of rock star to his society. The Jesse James of this telling is no Robin Hood robbing the rich to give to the poor, and that train robbery we witness is punctuated by acts of gratuitous brutality, not gallantry. Nineteen-year-old Bob Ford (Casey Affleck) seeks to join the James gang out of hero worship stoked by the dime novels he secretes under his bed, but his glam hero (Brad Pitt) is a monster who takes private glee in infecting his accomplices with his own paranoia, then murdering them for it. In the careful orchestration of James's final moments, there's even a hint that he takes satisfaction in his own demise.

Affleck and Pitt (who co-produced with Ridley Scott, among others) are mesmerizing in the title roles, but the movie is enriched by an exceptional supporting cast: Sam Shepard as Jesse's older, more stable brother Frank; Sam Rockwell as Bob Ford's own brother Charlie, whose post-assassination descent into madness is astonishing to behold; Paul Schneider, Garret Dillahunt, and Jeremy Renner as three variously doomed gang members; and Mary-Louise Parker, who as Jesse's wife Zee has few lines yet manages with looks and body language to invoke a wellnigh-novelistic backstory for herself. There are also electrifying cameos by James Carville, doing solid actorly work as the governor of Missouri; Ted Levine, as a lawman of antic spirit; and Nick Cave, composer of the film's score (with Warren Ellis) and screenwriter of the Aussie "Western" The Proposition, suddenly towering over a late scene to perform the folk song that set the terms for the book and movie's title.