1. Alfie (1966)
The opening scenes on the Embankment remain as iconic as miniskirts and Beatle haircuts in terms of 60s pop culture. Caine's assurance of delivery in the to-the-camera monologues keeps us with the character all through the movie, despite his more nefarious comings and goings.
2. The Ipcress File (1965)
The Kitchen Sink James Bond, Caine is the perfect choice to play Len Deighton's great antihero.
3. The Italian Job (1969)
Okay, the title gives it away: this film is not really set in London. The most memorable scene, thanks to Caine's handling of the film's best line, was shot in Crystal Palace Park. All together now, 1, 2, 3: "You were only supposed to blow the bloody doors off!"
4. Harry Brown (2009)
A modern vigilante classic in which Caine plays an ex-servicemen out to avenge his friend's death. Not Caine's easiest film to enjoy, London looks bleak and harrowing as a backdrop, but Caine's deft manipulation of the media brought the social problems inherent in the film into the news.
5. Jack the Ripper (1988)
This made-for-TV movie sees Caine tackle the role of Inspector Abberline, one of the London coppers given that task of cracking the Jack the Ripper case. A tough job, it's no wonder Caine's character takes a snifter or two. Or three.
POST UPDATED 6/4/16
A London Walk costs £10 – £8 concession. To join a London Walk, simply meet your guide at the designated tube station at the appointed time. Details of all London Walks can be found at www.walks.com.