The little girl looked on in awe as the Prince held his hand out for her to shake, before crouching down to pose for pictures.
The 29-year-old Prince was visiting Radio 2 to promote the upcoming Invictus Games, a paralympic-style sporting event for injured servicemen and women.
CLICK ON PICTURE FOR GALLERYHarry said: "I am hugely grateful to all the artists and organisers for coming together in September to put on what will be a truly awesome concert."
"It will be a celebration of everything the competitors will have achieved over the four days of the Invictus Games, not to mention the efforts of the hundreds of other athletes we couldn’t fit into the teams this year", he said, before adding: "And for those who didn’t make it back from operations, this is also for you."
The concert will see some of the world's biggest musicians perform at the ceremony, during which the medals will be handed out to winning athletes.
The Foo Fighters, Ellie Goulding, Kaiser Chiefs, James Blunt, Ryan Adams, The Vamps, hip-hop duo Rizzle Kicks, Britain’s Got Talent winners Diversity and the Military Wives Choirs will all perform.
The Games will see 300 competitors from around the world take part in events, which could include shooting, sitting volleyball, track and field and wheelchair basketball.
The aim of Harry's project is to encourage wounded servicemen to stay physically active when they return to their local communities and to introduce them to sporting challenges on a Paralympic level.