The Duke of Cambridge will also move his family to Kensington Palace in London from their current family base in Anmer Hall, Sandringham.
The 34-year-old has told East Anglian Air Ambulance (EAAA) that he will not be renewing his two-year contract with them when it lapses in a few months' time in the summer.
In a statement, Prince William said: "It has been a huge privilege to fly with the East Anglia Air Ambulance.
"I would like to thank the people of East Anglia for being so supportive of my role and for letting me get on with my job when they have seen me in the community or at our regions hospitals.
"I would especially like to thank all of my colleagues at EAAA, Babcock, and Cambridge Airport for friendship and support. I have loved being part of a team of professional, talented people that save lives every day.
William and Kate, Duchess of Cambridge, will make the move to London so that their children, Prince George and Princess Charlotte, can begin a new school and nursery, respectively, in the British capital.
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