The actor was pictured braving chilly winds as he stood at the top of the tower of the art gallery staring down an approaching helicopter.
Cruise, 55, who is known for performing his own stunts, last year injured himself when he jumped between two buildings during a shoot in the capital.
But he looked back to fighting fit in the scene, in which he looked as though his character, Ethan Hunt, was preparing to make a death-defying jump from the tower onto the helicopter.
The star had a safety harness strapped to his leg and looked to be in deep concentration as he filmed of the tense scene.
The dramatic pictures show Tom Cruise running across the rooftop, silhouetted in front of the London skyline.
He was also pictured running through the streets dressed in his character’s all-black outfit.
Last month, filming for the latest instalment of the popular action franchise brought parts of central London to standstill as Cruise filmed scene where he sprinted across the roof of Blackfriars Rail Bridge.
Cruise again braved bitterly cold conditions as he sprinted high over the Thames with a low-flying helicopter filming his progress.
And on Wednesday he was seen flying through the air as he was propelled by a harness off the roof of St Paul’s Cathedral.
Mission: Impossible – Fallout is due to be released in July.