Twelve fire engines and around 80 firefighters tackled a church fire on Hamilton Terrace in St John's Wood.
The whole of the two-storey building was destroyed by fire. There were no reports of any injuries.
The fire was producing a significant amount of smoke in the local area and residents were advised to keep their windows and doors closed.
Firefighters used two of the Brigade's new 32-metre turntable ladders and a 64-metre turntable ladder (the tallest in Europe) as water towers, to get water on to the building externally.
The Brigade's 999 Control Officers took more than 30 calls to the blaze.
The Brigade was called at 2319 and the fire was under control by 0222. Fire crews from North Kensington, Paddington, West Hampstead and surrounding fire stations attended the scene.
Due to the unsafe structure of the building, the cause of the fire has been recorded as undetermined.