Disagreements between secessionist parties, which gained a majority in last year’s regional polls, have blocked the formation of a Catalan government.
Catalonia’s acting leader said he supported the mayor of the Girona region, Carles Puigdemont, as his replacement.
Artur Mas i Gavarró has been in power since 2010.
In September elections, Artur Mas’ Junts pel Si (Together for Yes) alliance won 62 of the 135 seats in the Catalan assembly.
However, a small anti-capitalist and pro-independence party, the CUP (Popular Unity Candidacy), which holds 10 seats, has refused to support Artur Mas as leader.
“I am stepping aside and will not be standing as a Junts pel Si candidate for the re-election of president of the regional government,” Artur Mas told a news conference in Barcelona.
Nationally, Spain faces weeks of political uncertainty after an inconclusive general election on 20 December.
In November 2015, the Catalan parliament voted to start the secession process – a move declared unconstitutional by Spain’s conservative Popular Party (PP), which ran the country before last month’s election.
Catalonia is a highly industrialized and populous region in Spain’s north-east that accounts for about a fifth of the country’s economic output.
Both the PP and the Socialists (PSOE), who came first and second respectively in Spain’s general election, oppose Catalan secession.
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