The Australian was locked in an entertaining battle with Norway's Casper Ruud when the incident brought an abrupt end to the match in the third set.
Kyrgios led 2-1 with the deciding set going with serve when he received a game penalty for unsportsmanlike conduct having been broken for 1-1.
The 24-year-old proceeded to lob his chair onto the court before he packed his bag and walked off the court.
As a result, he was officially defaulted from the match and Ruud was declared the winner.
The incident comes a day after he branded Rafael Nadal a sore loser, the Spaniard's uncle Toni an "idiot" and said world number one Novak Djokovic has a "sick obsession" with being liked in a podcast ahead of the French Open.
Speaking to tennis writer Ben Rothenberg on the 'No Challenges Remaining' podcast, the 24-year-old also disparaged a number of other top professionals and fans who heckle him at his matches.
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The world number 36 labelled the French Open champion "super salty" and only gracious after victory.
"When he wins, it’s fine. He won’t say anything bad, he’ll credit the opponent, ‘He was a great player’. But as soon as I beat him, it’s just like, ‘He has no respect for me, my fans and no respect to the game’," said Kyrgios.
"It’s not a good look for you, I feel. And then uncle Toni came out saying, 'He lacks education'. I’m like, 'Bra (brother), I did 12 years at school, you idiot. I’m very educated. I understand that you’re upset I beat your family again’."
Kyrgios described Djokovic as "an unbelievable player" and "a champion of the sport" but said the Serb was too desperate to be admired like popular Swiss rival Roger Federer.
"I just feel like he has a sick obsession with wanting to be liked. He just wants to be like Roger," he said.
"For me personally - I don’t care right now, I’ve come this far - I feel like he just wants to be liked so much that I just can’t stand him.
"This whole celebration thing that he does after matches, it’s like so cringeworthy. It’s very cringeworthy."