In mid-1973, Cruyff was sold to Barcelona for 6 million guilders (approx. US$2 million, c. 1973) in a world record transfer fee. On 19 August 1973, he played his last match for Ajax where they defeated FC Amsterdam 6–1, the second match of the 1973–74 season.

Cruyff endeared himself to the Barcelona fans when he chose a Catalan name, Jordi, for his son. He helped the club win La Liga for the first time since 1960, defeating their deadliest rivals Real Madrid 5–0 at their home of the Santiago Bernabéu. Thousands of Barcelona fans who watched the match on television poured out of their homes to join in street celebrations. A New York Times journalist wrote that Cruyff had done more for the spirit of the Catalan people in 90 minutes than many politicians in years of struggle. Football historian Jimmy Burns stated, "with Cruyff, the team felt they couldn’t lose". He gave them speed, flexibility and a sense of themselves. In 1974 Cruyff was crowned European Footballer of the Year.

During his time at Barcelona, Cruyff scored one of his most famous goals, "The 'Phantom' Goal". In a game against Atlético Madrid, Cruyff leapt into the air, twisted his body so he was facing away from the goal, and kicked the ball past Miguel Reina in the Atlético goal with his right heel (the ball was at about neck height and had already travelled wide of the far post)