The former presenter and commentator’s new show will broadcast between 10am to 1pm every weekday from 14 February.
The appointment comes just weeks after Gray and Keys were recorded off-air making sexist comments about female assistant referee Sian Massey.
Both commentators have since apologised but Gray was subsequently sacked from Sky Sports and Keys resigned.
TalkSport’s programme director Moz Dee says the appointments are “great for the [radio] industry”.
Dee adds: “This continues our commitment to investing top talent and rights, and build on our recent RAJAR success and our biggest audience ever.”
TalkSport had 3.08 million listeners in the three months to 31 December, a 4.3% increase on the third quarter and up 23.7% on the same period last year, largely boosted by England’s Ashes victory and a competitive Premier League title race.