London Overground has signed a deal with The Cloud to provide free Wi-Fi to passengers at some 56 stations across the capital.
It will not be ready in time for the Olympic Games, however, as the rollout of the service will begin in the summer and be completed by the end of the year.
Access will be made available in the immediate vicinity of the station and users will have 60 minutes free internet access each day at each station following a one-time registration process.
According to London Overground, no extra cost will be placed on the taxpayer and no increase in fares will be required.
"Access to the internet is no longer limited solely to home or to the workplace, and people's expectation is to be able to work and communicate effectively and seamlessly while they're on the move so we're delighted to support this initiative which will bring reliable, free Wi-Fi to London Overground's customers," said Steve Murphy, managing director of London Overground.
Some of the stations set to benefit from the service before the end of 2012 include Willesden Junction, West Hampstead, New Cross Gate, Forest Hill, West Croydon, Surrey Quays, Dalston, Wapping and Shepherd's Bush.
The announcement follows recent news that Virgin Media has been selected by London Underground to offer free Wi-Fi in 80 of the capital's tube stations in time for the summer's Olympic Games.
The underground service will be made available throughout the selected stations, on the platforms and offer speeds comparable to 4G, according to Virgin.
Passengers will only lose connectivity when going through the tunnels, but will automatically reconnect as the tube pulls into the platform.
However, following the Olympic and Paralympic Games full internet access via Wi-Fi in the underground stations will be chargeable on a pay-as-you-go basis, but users will still be able to connect and view Transport for London (TfL) travel information.