Lunts will oversee planning, housing, the Thames Gateway, the Olympic bid and the Architecture and Urbanism Unit.
Lunts has joined the GLA from the ODPM, where he was the director of urban policy and worked closely with the deputy prime minister developing many aspects of the Sustainable Communities Plan.
Lunts was the chief executive of the Prince' Foundation from 1998 until 2002, where he worked on projects such as the Ancoats Urban Village in Manchester.
Mayor Ken Livingstone said he was delighted to have recruited Lunts to his team. 'David has a record of innovation in the public policy field,' he said. 'He brings together a wide experience of both policy work and frontline project delivery.
'He is well respected in both the public and private sectors and I'm sure he will make a tremendous contribution to our work at City Hall. I look forward to working with him,' Livingstone added.