The team of five men and one woman set off from their starting base in Moray, Scotland, at 11am on Saturday.
The six, who all have either physical or cognitive injuries sustained in the line of duty, are expected to clock up hundreds of miles over 72 days as they travel south to England and Wales to reach their final destination of London and Buckingham Palace on November 1.
The Walk of Britain is designed to raise awareness of the work of the charity Walking With The Wounded, which supports injured members of the armed forces back into independence through employment.
The core team of four British and two US wounded veterans will be joined by other wounded personnel each week in different parts of the country.
The team began their trek from the Glenfiddich Distillery in Dufftown.
The first week of the walk will take them to the likes of Loch Ness, Fort William, Pitlochry, Scone Palace and the Falkirk Wheel, as well as Glasgow and Edinburgh.
The trek through mainland UK will eventually see them reach the summit of four peaks - Ben Nevis, Scafell Pike, Snowdon and Pen Y Fan.
Edward Parker, co-founder of the charity, said: ''Walking over 1,000 miles is no mean feat. Yet again, we will be able to demonstrate that despite injuries these men and women look to their future with great determination and courage.
''We are also very excited about walking amongst the communities who have been so supportive of the military and Walking With The Wounded and we look forward to them coming out to support the team on their journey.''
Richard Waite, chairman of Esri UK, the company sponsoring the first week of the walk, said: "We are immensely proud to support these young men and women who have given so much to their countries through active service."
The challenge was launched earlier this year at a reception attended by Prince Harry, who announced he would join the group for a ''small part'' of their journey.
Harry has supported the charity since it was formed, taking part in a trek to the North Pole in 2011 and South Pole in 2013. He was also patron of its Everest expedition in 2012.
During his 10-year full-time military career, he went on two tours of duty to Afghanistan and qualified as an Apache aircraft commander.
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