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TfL (and therefore the Mayor) control TLRN roads, which are the ones with double red lines instead of yellow. These make up about 4% of London’s roads and tend to be bigger arterial ones. The 32 boroughs and the City of London control the rest.
The Mayor could build Cycle Superhighways on TLRN tomorrow, in theory, but has to get council approval for any changes to borough roads.
Sparky
From the sound of things the majority of roads are under the control of the council and the mayor doesn't have the power to force them to do anything.