Dembélé made his debut on 9 September as a 68th-minute substitute for Gerard Deulofeu in a 5–0 Derbi barceloní win over Espanyol at the Camp Nou, assisting the final goal by Luis Suárez. In his first league start eight days later at Getafe, he injured his hamstring and was ruled out for four months. He was given the medical all-clear on 2 January 2018, but a couple weeks later, he again injured himself against Real Sociedad and was ruled out for up to four weeks. On 14 March 2018, Dembélé scored his first goal for Barcelona, netting the second goal in a 3–0 second leg win in the Champions League round of 16 against Chelsea. On 17 April, he scored his first La Liga goal for Barcelona, notching the opening goal in an eventual 2–2 draw with Celta Vigo. On 9 May, Dembélé scored twice, marking the first brace of his Blaugrana career, in a 5–1 home victory over Villarreal. Dembélé won both the Copa del Rey and La Liga winners' medals in his first season in Spain, with the 20-year-old scoring four goals in 24 appearances across all competitions.
On 12 August 2018, Dembélé scored the winning goal against Sevilla in the Spanish Super Cup, in an eventual 2–1 victory to win Barcelona their 13th Supercopa de España title. He opened his La Liga season's goal tally by scoring the only goal of the game against Real Valladolid, on 25 August, away at the José Zorrilla. A week later, on 2 September, Dembélé notched his first home goal of the season, as the Blaugrana demolished newly promoted Huesca 8–2. Dembélé was again on the scoresheet the very next game, on 15 September, netting his third match winner of the ongoing campaign in a 2–1 away victory over Real Sociedad at the Anoeta. On 18 September, Dembélé scored his first Champions League goal of the season, helping Barça defeat PSV Eindhoven 4–0 at the Camp Nou. Coming on as a substitute against Real Madrid, on 28 October, Dembélé set up Arturo Vidal's last goal of the game in a 5–1 home El Clásico triumph. Just a week later, again appearing from a bench role, he inspired Barcelona to a 3–2 comeback away against Rayo Vallecano, scoring the 2–2 equalizer with a half-volley in the 87th minute.
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.