The move is part of a review undertaken by Lawn Tennis Association (LTA) chief executive Michael Downey.
Britain's Davis and Fed Cup teams, the wheelchair programme and junior training camps will remain at the NTC.
The Roehampton venue opened in 2007 at an estimated cost of £39m, and is also the administrative base of the LTA.
Responding to a report in The Telegraph, an LTA statement said: "Most of the high-performance players who were part of the national programme and based at the NTC are making plans to relocate to high-performance centres."
Former British number one Laura Robson is currently using the NTC as she recovers from a wrist injury, and an LTA statement said the facility would continue to serve as "a drop-in centre for Britain's professional players".
Robson wrote on Twitter: "I think a few of the Fed & Davis cup team members plan to stay as it's closest to our homes/physios are based at NTC."
With 16 outdoor and six indoor courts, a gymnasium and sports science and medical facilities, as well as accommodation, it was hoped the facility in south-west London would help produce world-class players.
However, seven years on, Britain has just two top-100 players in Andy Murray and Heather Watson, neither of whom came through the NTC.
Bob Brett, formerly coach to Boris Becker and Goran Ivanisevic among others, will take up the role of head of player development next month and has already submitted a report on the structure of elite tennis in the UK.
Britain's leading players will not be based at the National Tennis Centre (NTC) in future, relocating instead to high-performance centres around the UK.