Walking routes in Croydon are to receive a share of a £30million grant from the London Assembly.
Sutton and Merton will also benefit from a plan to redevelop existing pedestrian facilities and lay lots more.
The aim is to lower emissions and to get more people walking their way to a healthier lifestyle.
London Mayor Ken Livingstone said: "The expansion of cycling and walking will help reduce our impact on climate change and reduce traffic congestion.
"About 20 per cent of the carbon emissions savings we've calculated we can make from transport by 2025 will come from changing the way we travel.
"We know Londoners want the opportunity to walk and cycle more. One in two people say they want to walk for short journeys where they currently use their car."
Funding is being earmarked for the development of more than 100 new projects, including linking existing walking routes and expanding pedestrian zones.
Green Party Assembly Member Jenny Jones said: "London's pedestrians are finally getting the investment they deserve.
"The great projects that have been funded this year show how this extra money is badly needed.
"With funding in place until 2010, walking in London is finally on the front foot."
Crossings, bridges and footpaths are to be overhauled and new leisure walks to be created over the next two years.
A Croydon Council spokesman said: "Since 2004, Croydon Council has received £625,000 from Transport for London to fund a scheme designed to improve walking routes in the south Wandle area. The scheme is set for further enhancement over the next financial year with a further cash injection of £150,000. It ties in with the Sustrans Connect2 project that expands the Wandle Links network.
"This is great news for people in the area, whether they walk for leisure or for more prosaic reasons, such as shopping or getting to work.
"The links this project have already provided, and those it will yet support, are a real boon, allowing walkers to enjoy the fresh air and reap the health benefits that ensue."
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