At Grêmio, Paulo Nunes lived the most glorious time in career, winning two Campeonato Gaúcho titles, the Copa Libertadores cup, the Campeonato Brasileiro, the Recopa Sul-Americana and the Copa do Brasil for the Porto Alegre team and being the lead scorer in the 1996 Campeonato Brasileiro and the 1997 Copa do Brasil. His good form also earned him the Bola de Prata from "Placar" magazine, also earning him a place in the national team squad for the 1997 Copa América.