Carlos Alberto started his career with Fluminense, where he won the Campeonato Carioca in 2002. He moved on to FC Porto under coach José Mourinho in January 2004. There, he won the Portuguese Championship and the UEFA Champions League, where he scored the first goal in the 3–0 win over AS Monaco in the final match. In the beginning of 2005, he moved to Corinthians who signed a partnership with MSI, where he won the Brasileirão in 2005 being one of the major players of the team. In 2006 Corinthians did poorly in all competitions and Carlos Alberto lost a lot of room in the team and after a long fight with Corinthians manager Emerson Leão, which peaked at a Copa Sul-Americana game against Club Atlético Lanús. He stated he would never again play in Corinthians as long as Leão remained as manager. He was loaned out to Fluminense from January to December 2007, being the team captain in their Copa do Brasil title. He joined Werder Bremen in July 2007 with a deal of reported €7.8m which was a club record. He signed a four-year contract. The move did not work out for either club or player however, as he suffered with insomnia, and returned to Brazil on numerous loan spells. In January 2008 he was loaned out to São Paulo but he was excluded from the squad for disciplinary reasons in April 2008 three months before his contract ended. In May 2008, he signed another loan contract with Botafogo until June 2009 but on 12 November 2008, he left the club because of outstanding salary payments. On 7 January2009, he was loaned out yet again, this time to CR Vasco da Gama for 6 months until 30 June 2009. Later he signed for another year on loan with Vasco da Gama. In June 2010 his contract with Werder Bremen was mutually terminated. He signed a three-year contract with Vasco da Gama until June 2013. On 14 January 2015, Carlos Alberto joined Emirati club Al Dhafra on a one-year contract. 15 days later, however, the move collapsed and he returned to Brazil. On 24 April 2015, he joined Figueirense along with Felipe. On 13 January 2017, he signed a one-year contract with Atlético Paranaense. In 2019, after being without a club for a year, Carlos Alberto joined Boavista playing in the Campeonato Carioca. In June 2019, he announced his retirement.
