Pujol was captured in 1960 and detained for his protests against the regime of Francisco Franco. He was sentenced to seven years in prison, accused of organizing the opposition campaign. However he got out after spending only two and a half years in jail, and immediately started a new line of political activity with the slogan "building the country". This aimed to raise Catalans' national awareness and create the necessary cultural and financial institutions for the development of Catalonia.
In 1974, he passed definitively to the political sphere on founding the political party called Convergència Democràtica de Catalunya (Democratic Convergence of Catalonia), of which he was the first Secretary.
He was elected as the president of Catalonia (Generalidad de Cataluña) in 1980, and reelected again in 1984, 1988, 1992, 1995 and 1999.
Pujol retired in 2003, leaving the head of the party (CDC) to Artur Mas.