One of the game's bright young prospects, the 20-year-old Australian wrote on his website that the decision was mutual and the pair would remain friends.
Larkham worked with Kyrgios in his junior days and was in a second stint with the Australian after he parted ways with former coach Simon Rea after Wimbledon last year.
"It's never an easy decision to end a coaching relationship and to do so prior to the start of a grand slam is even more difficult," said Kyrgios, a quarter-finalist at Wimbledon last year and at his home Grand Slam in January.
"But I feel that this is the right decision for me at this time. I will work closely with my team and Tennis Australia through Wimbledon and we will regroup after the tournament in order to figure out the best plan for the future."
The rangy world number 29 has had a mixed season since his run to the quarters at Melbourne Park, making his first ATP final at Estoril but also being troubled by an elbow problem.
Kyrgios withdrew from a tournament in Stuttgart earlier this month due to the elbow and pulled out of the Nottingham warm-up for Wimbledon citing illness.
Wimbledon starts on Monday.
Image: Nick Kyrgios
Photograph: Clive Brunskill/Getty Images