Speaking after a two-and-a-half-hour meeting with Mariano Rajoy, Catalonia president Artur Mas said although there was no agreement on the referendum issue, there was a willingness on both sides to keep talking and that was positive.
Mr Mas said Catalonia wants the November 9 referendum to be held legally and, if possible, with Madrid's blessing.
The independence campaign holds profound consequences for Spain as it emerges from a severe economic crisis. Europe will be watching the debate closely, along with Scotland's independence referendum in September.
A Spanish government statement said Mr Rajoy had reiterated to Mr Mas the planned referendum was illegal and would be blocked.
Mr Rajoy said the most important thing right now for all of Spain, including Catalonia, was to consolidate the recovery from a severe economic crisis the country has endured since 2008, which has seen unemployment levels soar to 25 per cent.
The closed-door session between the two political leaders followed months of clamour by political parties and business groups for the two to sit down and try to come up with a framework to prevent the dispute from boiling over.
Pro-independence sentiment in Catalonia has grown greatly in recent years, fuelled by a sense the region deserves better economic and political treatment from Madrid.
In the proposed November referendum, the regional government wants to ask voters if they want Catalonia to be a state and, if so, should it be independent.
Polls show that while a strong majority of Catalonia's 7.5 million residents want the ballot, only about half favour severing ties.
Mr Mas believes a win for the Yes vote in Scotland could boost Catalonia's bid for independence.