A major incident was triggered by the horror crash after the chopper hit the structure by the St George Wharf Tower development in Vauxhall close to the river Thames at 8am.
The stricken helicopter then turned into a "fireball" and "spiralled into the ground", said shocked onlookers.
Part of the damaged crane is understood to have then hurtled to the ground, smashing into a neighbouring building.
Horrifying footage shows what looks like burning helicopter fuel covering the road around a crashed motorbike.
And lifeboat crews are searching the Thames after possible sighting of a person in river after the crash.
Astonishing reports on London radio station LBC also said the driver of the crane was LATE for work - otherwise he would have been in the crane at the time of the crash.
The Metropolitan Police said two people died at the scene and two had been taken to hospital.
London Fire Brigade said firefighters had rescued a man from a burning car and he was taken to hospital by London Ambulance Service crews.
A pall of smoke was visible near the River Thames at the scene, which is close to the MI6 building and the new American embassy which is under construction.
But government sources say the crash “has nothing to do with nearby MI6”.
Reports say there was one person in the helicopter - believed to be an Augusta 109 - and that cars were damaged on the road. Other cars are seen on fire.
Conservative MP Nicky Morgan was walking towards Vauxhall when the accident happened.
She told BBC News: "Within a minute there were sirens, so you felt that the emergency services were immediately reacting, which was comforting. It is a terrible, unexpected tragedy. I wondered if it was a bomb explosion."
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