
The movie, which features the star as a killer fighting an epidemic of the undead, took $25m (£15.7m) in its opening weekend.
Harrelson's previous best opening was 1993's Indecent Proposal which took $18m (£11.3m)
Family animation Cloudy With a Chance of Meatballs slipped to number two.
The top 10 featured four other new releases in a weekend where sales were generally down.
US BOX OFFICE TOP FIVE
1 Zombieland -$25m
2 Cloudy With A Chance of Meatballs - $24.6m
3 Toy Story & Toy Story 2 3D - $12.5m
4 The Invention of Lying -$7.4m
5 The Surrogates - $7.3m
Source: Hollywood.com
A 3D double-feature re-issue of Pixar's Toy Story and Toy Story 2 opened at three with $12.5m (£7.4m), ahead of the release of Toy Story 3 in 3D next June.
Ricky Gervais comedy The Invention of Lying, which takes place in an alternate reality where everyone tells the truth, debuted at number four.
Michael Moore's Capitalism: A Love Story took $4.85m (£3m) despite only showing in 962 cinemas.
It tied in sixth place with Drew Barrymore's directorial feature debut Whip It starring Ellen Page as a teenager who attempts to escape small town life by taking up roller derby, a contact sport of speed roller skating.