Thuram and Zambrotta faced each other in the World Cup final
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Barcelona have won the race to capture Juventus defenders Lilian Thuram and Gianluca Zambrotta following the Italian club's relegation to Serie B.
Thuram, 34, has signed a two-year deal, while the 29-year-old Zambrotta has put pen to paper on a four-year contract.
Juventus were relegated and will start next season with a 30-point penalty after the match-fixing scandal which rocked Italian football.
Spanish media reports suggest Barca have paid a combined fee of £13m.
The pair will join their new team-mates on Barca's tour of Mexico and the USA.
France's Thuram and Italy's Zambrotta both enjoyed outstanding tournaments in the World Cup, facing each other in the final.
Thuram, who has also had spells with Monaco and Parma, was part of the France squad which won the 1998 World Cup and Euro 2000.
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He won 121 caps for France before calling an end to his international career after his country's defeat to Italy on penalties in the final.
Meanwhile, Zambrotta - who can also play full-back on either flank - spent two seasons with Bari before moving to Juventus in 1999. He has 58 caps for Italy.
Thuram's spokesman told BBC Sport earlier this week that the veteran defender had been in heavy demand from top clubs throughout Europe.
"Clubs like Barcelona, Real Madrid, AC Milan, Arsenal and Chelsea have been asking about Lilian," he said.
Many star players are expected to leave Juventus, Milan, Lazio and Fiorentina in the wake of Italy's match-fixing scandal.
Juventus lost Italy's World Cup-winning captain Fabio Cannavaro and Brazil midfielder Emerson to Real Madrid on Wednesday.