Dembélé was born in Vernon, Eure, in Normandy. His mother is French of Mauritanian and Senegalese descent, while his father is from Mali. He took his first footballing steps in nearby Évreux, first at ALM Évreux and then at Évreux FC 27 between the ages of 12 and 13.

Dembélé was called up to the senior France squad for the first time to face Italy and Belarus in August 2016 after Alexandre Lacazette and Nabil Fekir withdrew through injury. He made his debut on 1 September against the former at the Stadio San Nicola, replacing Antoine Griezmann for the final 27 minutes of a 3–1 friendly win over Italy. On 13 June 2017, Dembélé scored his first France goal in a 3–2 friendly victory against England.

On 17 May 2018, he was called up to the 23-man French squad for the 2018 World Cup in Russia.On 15 July, he was an unused substitute, as France beat Croatia 4–2 in the final.

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