Bank, Oxford Circus, Tottenham Court Road, Euston, and Camden Town will gain coverage following a successful pilot scheme on the eastern end of the Jubilee line.
Mobile phone reception has been available on the eastern half of the Jubilee line since March 2021.
All major mobile phone networks have signed up to provide coverage across the Tube network, TfL said.
TfL has awarded a 20-year deal to 4G and 5G infrastructure company BAI Communications to deliver the project.
Once complete, customers will be able to make calls and access the internet wherever they are in the five stations.
Once those first five stations are live, TfL says that further sections of the tube network will go live by summer 2023 – including stations across the City and West End on the Central line.
TfL and BAI are also continuing to progress with delivering mobile coverage across the recently opened central section of the Elizabeth line between Paddington and Abbey Wood.
Plans are in motion for the entire London underground to have full mobile phone coverage by 2024.
The mayor of London, Sadiq Khan, said: “Improving the capital’s connectivity and digital infrastructure is central to London’s economic recovery from the pandemic, so I am delighted that Vodafone and Virgin Media O2 customers will now have access to high-speed mobile coverage when travelling on the Tube.
“I committed to Londoners that I would deliver 4G throughout the Tube network as part of my determination to build a better London for everyone – and I have no doubt that this will transform journeys for millions of passengers.”
Shashi Verma, chief technology officer at TfL, said: “Mobile connectivity across the stations and tunnels across the Tube network will help our customers stay connected more easily as well as work, shop and stay in touch on the move.
“I’m delighted that all four major mobile operators are set to provide high-speed, uninterrupted 4G coverage on the Tube.
“We are working hard with BAI Communications to get the next stations completed by the end of the year so our customers can benefit as soon as possible.”