The defending women's champion Angelique Kerber would also suffer elimination today.

Murray had emerged as the clear favourite to win the Grand Slam for the first time in his career after Serbia’s Novak Djokovic, who had beaten him four times in the final, suffered an early exit.

The Briton would instead join Djokovic on the list of eliminated players, with an inspired Zverev producing a superb display.

Zverev, the world number 50, would raise the prospect of an upset by triumphing 7-5 in the opening set of the contest.

The world number one would respond by claiming the second set by the same scoreline, but Murray continued to struggle against Zverev’s serve and volley tactics.

Zverev, whose younger brother Alexander was beaten by Spain’s Rafael Nadal yesterday, would triumph in the next two sets to secure a shock 7-5, 5-7, 6-2, 6-4 win.

"Just wasn't meant to be," said Murray, who was broken eight times in the contest.

"He served very well when he needed to, especially when he was behind in games.

"He deserved to win because he played great when he was down, and also in the important moments.

"I was kind of behind in the last couple of sets the whole way, but the first two sets, I had chances.

"I was up a break I think in both of them pretty early, but couldn't convert my opportunities."

Britain’s challenge in the men’s singles is now at an end, as France’s Jo-Wilfried Tsonga overcame Dan Evans 6-7, 6-2, 6-4, 6-4.

Murray’s defeat, though, was the main talking point of the day as the title now appears up for grabs for a number of players.

Switzerland’s Roger Federer could be one man to benefit as the 35-year-old, a four-time winner of the tournament, came through a tough five set match with Japan’s Kei Nishikori by a 6-7, 6-4, 6-1, 4-6, 6-3 scoreline.

His compatriot Stanislas Wawrinka also reached the quarter-finals, with the 2014 winner beating Italy’s Andreas Seppi 7-6, 7-6, 7-6.

In the women’s singles, Kerber would falter in the last 16 as the German fell to defeat against America’s Coco Vandeweghe.

The defending champion had struggled through the early rounds of the tournament, but the world number one managed to battle through.

Her title defence would be ended by Vandeweghe though, with the American securing a 6-2, 6-3 win.

She will face Spain's seventh seed Garbine Muguruza in the quarter-finals, after the reigning French Open champion won 6-2, 6-3 against Romania’s Sorana Cirstea.

America’s Venus Williams was among the big-name winners as the seven-time Grand Slam champion secured a straight sets 6-3, 7-5 win over Germany's Mona Barthel.

She will now take on Russia’s Anastasia Pavlyuchenkova, who overcame her compatriot Svetlana Kuznetsova in their last 16 match.