The youthful prince, who played the sport at school and is a qualified rugby coach, eagerly got involved as he was pictured darting around the Twickenham green.
While Harry showed off his impressive skill set, England World Cup winner Jason Robinson assisted the royal in the training session, and joked that Harry could try out for the national team.
"We're looking for a winger or a full-back," said Jason. "I'll be looking to see what you've got."
"I think I'm a bit past it already," replied a modest Harry.
Looking every inch the sporting professional, Harry wore a white polo shirt and black tracksuit bottoms as he threw himself into the game. The charming royal entered into the competitive spirit as he joked around and jostled the ball from Jason, while cheering on the eager students.
"It's just fantastic to see him out here with the kids," said Jason. "He's dripping with sweat. He's put everything into this, because he is passionate about the game."
As patron of the Rugby Football Union All Schools Programme, Harry held the session for state school pupils in the hope of encouraging more students to get into the sport and join their local clubs.
This is not the first time Harry has taken part in rugby training sessions. On his visit to Brazil last year, the fun-loving Prince played a game of rugby in the sand with children from the slums of Rio de Janeiro.
After his session at Twickenham, Harry will head to Imperial College in central London to officially open the Royal British Legion Centre for Blast Injury Studies. The royal will be given a tour of the facility and is expected to deliver a speech.