Under Larsen, who took up the selector's role in 2015, New Zealand enjoyed tremendous success across formats, including reaching the finals of the 2019 50-over World Cup and 2021 T20 World Cup, and winning the inaugural World Test Championship (WTC) in 2021.
"The past seven-and-a-half years have just flown by and I've relished and enjoyed every minute of it," Larsen said in an NZC media release.
"The discussions and deliberations have always been robust and challenging but my enduring memory will always be the quality of the people I've worked with - from high performance right through to the administration."
Larsen will be overseeing both the men's and women's high performance programmes at Warwickshire.
"WCCC is a club with an amazing history and tradition and I'm looking forward to joining the team and helping to drive the club's ongoing success," Larsen said. "I have a number of great memories of playing at Edgbaston during my New Zealand playing days and the atmosphere was simply terrific."
NZC's GM High Performance Bryan Stronach spoke highly of Larsen's contribution to New Zealand cricket as a selector.
"Gavin was part of a support team that made a key contribution to arguably the most successful period in the history of the New Zealand men's team," Stronach said.
"His appointment at Edgbaston reflects the respect in which he's held around the cricketing world."
Stronach added that the process to find a new selector will begin in due course.