Francis Ford Coppola's 1979 drama about the Vietnam war topped a survey based on previous recipients of the best film prizes the Circle hands out each year.
Schindler's List came second in the poll, with Oscar-winning German drama The Lives of Others coming third.
The poll was held to celebrate the 30th anniversary of the London Film Critics Awards, held every February.
Coppola's film was voted the best previous winner in a poll that took in all the recipients of the circle's best film, best British film and best foreign language film awards.
Based on Joseph Conrad's novella Heart of Darkness, the acclaimed film starred Martin Sheen, Robert Duvall and the late Marlon Brando.
Apocalypse Now was named best film at the first London Film Critics Awards, held in 1980.
Chairman Jason Solomons said he was "delighted" that "such a powerful and brilliant film has won the enduring admiration of the London critics".
The next London Film Critics Awards will be held on 18 February 2010, with proceeds going to the NSPCC.
The London Critics' Circle has more than 100 members who write for newspapers, magazines and websites all over the United Kingdom.
Another war movie, Kathryn Bigelow's The Hurt Locker, was the main winner at the Gotham awards, given out each year to US independent films.
The film, about bomb disposal experts stationed in Iraq, won best feature on Monday at the New York event, with an additional prize going to its actors Anthony Mackie, Jeremy Renner and Brian Geraghty.
Bigelow received a special tribute at the event, which focuses on low-budget films directed or produced by film-makers born or based in the US.
Food, Inc. - a documentary about the US food industry's impact on public health, animal rights and the environment - was named best documentary.
- 1. Apocalypse Now
- 2. Schindler's List
- 3. The Lives of Others
- 4. Unforgiven
- 5. Brokeback Mountain
