The Serb then lost in the bronze-medal match to Pablo Carreno Busta, before withdrawing from the mixed doubles and leaving the Japanese capital empty handed.
More than his tennis, it was the Serb's emotional outbursts that stole the headlines at the Olympics. During his loss to Carreno Busta, Djokovic smashed his racquet multiple times and even threw it into the empty stands after losing a point.
Weighing in on the matter, two-time Grand Slam champion Tracy Austin admitted that it was strange to see a top player like Djokovic lose control in such a fashion.
"First of all, Djokovic imploding, I have never seen a player where they actually kind of hit the ball in the net and take the racket and chuck it 15 rows up into the stadium," Austin told Tennis Channel.
"I will say, for Djokovic, he’s being compared to Federer and Nadal; these are like Mother Teresa and the Dalai Lama (of tennis). I mean, you know, they don’t do anything wrong. If he played in the era of John McEnroe, Ilie Nastase, and Jimmy Connors, he’d be number four," she added.
"It is never easy when Novak Djokovic is the target all the time" - Tracy Austin
During the interaction, Tracy Austin said she understood why Djokovic might have reacted the way he did as he was under tremendous pressure in his quest to achieve the Golden Slam.
"You know, he’s a perfectionist, he has his outbursts, he doesn’t love it either. He is not perfect, he is not great, but it’s never easy when he’s the target all the time," Austin said.
"He’s number one in the world, I am not condoning it. He has a lot of pressure. He was going for the ‘Golden Slam’," she added.
Rafael Nadal also recently commented on Djokovic's tendency to smash racquets. The Spaniard said he found it "strange" that someone as successful as the Serb could react in that manner, but attributed it to Djokovic's competitive streak.
"In the end he is number one in the world and one of the best in history," Nadal said. "It is strange that someone, being so successful, reacts in this way from time to time, but in the end he is very competitive and reacts like this."
Despite his Golden Slam hopes now over, Djokovic still has a lot to play for this year. Having won the Australian Open, Roland Garros, and Wimbledon titles already, the Serb can complete the Calendar Slam by lifting the US Open trophy this year.
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Winning in Flushing Meadows will make him the first man to achieve the Calendar Slam since Rod Laver in 1969. He will move ahead of both Roger Federer and Rafael Nadal in the all-time Slam race.