The 50-year-old actor plays an army lieutenant fighting an alien invasion in the science fiction action film, based on a Japanese novel of the same name, reported Digital Spy online.
A scene involving a Royal Air Force helicopter landing in the middle of Trafalgar Square forced the usually bustling public space to be shut down for shooting.
The "Mission: Impossible" actor was spotted stepping on the set clad in a sleek green military uniform complete with aviator sunglasses.
A number of extras dressed in khaki ponchos over camouflage uniforms were also spotted flocking on the set. Several tanks were also situated throughout the set.
"All You Need Is Kill" is scheduled for release in cinemas in March 2014.