[1] Simplício made his Serie A debut on 22 September 2004 in a 1–2 home loss against Bologna FC 1909, one day shy of his 25th birthday (16 minutes played), and finished his first season with four goals in 34 games, bettering that total to ten in the following campaign.

On 14 June 2006 Simplício joined fellow top division side U.S. Città di Palermo, moving alongside Parma teammate Mark Bresciano.

In January 2010, his agent Gilmar Rinaldi announced he would not extend his contract with Palermo, set to expire in June.

[6] He scored four league goals from 24 appearances in his debut campaign, adding the 2–1 winner against S.S. Lazio for the Coppa Italia as the capital side reached the semifinals.

[7] In 2011–12, Simplício netted the same number of goals, including one in a Derby del Sole against SSC Napoli in a 3–1 away triumph,[8] but Roma could only finish seventh, thus not qualifying for any European competition.