The Israeli's contract expired after the 2017 Africa Cup of Nations, where Ghana finished fourth, and there will be no renewal as the 62-year-old seeks pastures new.
"I've hugely enjoyed my time in Ghana taking over after the disastrous 2014 World Cup campaign and rebuilding the squad to reach the final in the African Cup of Nations for only the second time in 23 years, and also the semi-final of this year's competition," Grant said in a statement.
"And the passion and loyalty of the supporters is something I'll always remember."
Grant took control of the Black Stars in November 2014 and led the side to the 2016 Africa Cup of Nations final, but they exited this year's competition in the semi-finals.
The Ghana FA's president Kwesi Nyantakyi has reportedly already begun the search for Grant's successor.