On 26 August 2015, Tolói was signed by Atalanta B.C. for a €3.5 million transfer fee. He made his debut on 13 September, in a 2–2 league draw at Sassuolo, replacing Gianpaolo Bellini in the 80th minute. In his second match, eleven days later, he started and scored the sole goal, settling a 1–0 league win at Empoli.