The West Africans finished bottom of Group C after losing all three games, with a 3-2 defeat by Cameroon on Tuesday rounding off their campaign.
Tom Saintfiet resigned as coach of The Gambia after the Scorpions suffered a group-stage exit from the 2023 Africa Cup of Nations.
Saintfiet was appointed in 2018 and led the side to the quarter-finals of the 2021 edition of Afcon on their debut.
However, the Belgian could not repeat those heroics in Ivory Coast.
“Thank you for your service gaffer. Gambia will indeed miss a great tactician,” the Gambia Football Federation said in a message posted on X.
The Gambia were 168th in the world rankings when Saintfiet took charge in July 2018, and the 50-year-old departs after improving their position to 126th.
The Scorpions were the lowest-ranked team at the 2021 finals but beat Mauritania, Tunisia and Guinea on the way to the last eight, where they were beaten 2-0 by hosts Cameroon.
They opened their 2023 Afcon campaign with a 3-0 defeat by defending champions Senegal and then fell to a 1-0 loss against fellow West Africans Guinea.
Saintfiet has coached national sides in four different Fifa confederations and has extensive experience in Africa having previously managed Namibia, Zimbabwe, Ethiopia, Malawi and Togo.
The Gambia endured a difficult build-up to this year’s finals in Ivory Coast, with the squad caught up in last September’s devastating earthquake in the Moroccan city of Marrakesh, when over 2,000 people died, before their final qualifier against Congo-Brazzaville.
The squad boycotted a pre-tournament training session earlier this month while demanding a bonus payment for qualifying, and then saw their flight from Banjul to Ivory Coast aborted because of a pressurisation issue in the cabin.
Saintfiet claimed the travelling party “could have died” had the plane not turned back and landed just minutes after leaving the Gambian capital.