Nicholas Holgate, chief executive of Kensington and Chelsea council, said he was forced out by Prime Minister Theresa May's government after the blaze at the 24 storey Grenfell Tower.
Holgate said in a statement the Communities minister Sajid Javid had required the leader of the council, Nicholas Paget Brown, to seek his resignation.
"Despite my wish to have continued, in very challenging circumstances, to lead on the executive responsibilities of the Council, I have decided that it is better to step down from my role, once an appropriate successor has been appointed," Holgate said.
On Wednesday, May said support for families in the initial hours after the fire was not good enough.
"That was a failure of the state, local and national, to help people when they needed it most," she told parliament.
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