In the early 1960s, he worked as a freelance arranger for Odeon Records. He wrote arrangements for Wilson Simonal, Marcos Valle, and for his debut album, "Inútil Paisagem" (1964), which was dedicated to the work of Antônio Carlos Jobim and recorded in Rio when Deodato was twenty-two. Jobim praised him in the album's liner notes. Deodato played piano alongside guitarists Oscar Castro-Neves and Roberto Menescal. He has been credited for helping to start the career of Milton Nascimento. He was part of a committee tasked with choosing songs for a festival, and Deodato chose three by Nascimento.