The long-term contracts cover London Underground and London bus shelters. They are currently held by Viacom Outdoor and Adshel respectively.
TfL believes ad revenues have not increased in line with the outdoor market, which has grown by 75% over the past decade.
TfL group marketing director Chris Townsend said he is looking for 'a significant increase' in revenue, which will be used to fund public transport improvements and marketing.
TfL is also considering merging all its advertising estates into one sales house for the first time.
Townsend joined the transport body 18 months ago from Telewest, where he was director of interactive TV. His remit is to maximise the value of the contracts, which currently bring in £200m a year in ad revenue.