Mr Puigdemont fled to Brussels after Spanish authorities levelled charges of sedition, rebellion and misuse of public funds against him for his role in the region's disputed independence referendum.
The separatists' agreement is the first significant step toward forming a new government in the restive Spanish region following regional elections December 21.
Pro-independence parties secured a slim majority of seats but failed to win more than 50 percent of the popular vote, meaning there is still no end in sight to the months-long, and increasingly bitter, impasse.
The result was a setback for Prime Minister Mariano Rajoy of Spain, who had called the election in the hope that voters would deliver a decisive blow to the secessionist movement.
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A spokesman with Puigdemont's Junts per Catalunya (Together for Catalonia) ticket said that the separatist politician secured the backing of the left-republican ERC party Tuesday evening in Brussels. "The presidential candidate will evidently be Puigdemont", Junts pel Catalunya representative Jordi Xucla told Spanish national radio.
However, it is unclear how Mr Puigdemont would lead the regional government from Brussels as he could be arrested if he returns to Spain. Puigdemont became the independence movement's leader but is now a fugitive in Belgium.
He is in Belgium, however, and will be arrested if he comes back to Spain on charges of rebellion and sedition.
"It's evident that for governing Catalonia you have to be in Catalonia, you can't do that via WhatsApp or as a hologram", said Ines Arrimadas, the leader of the anti-independence Ciutadans (Citizens) party.
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The other main potential candidate to represent the pro-independence parties would be ERC leader Oriol Junqueras, who is serving a custodial sentence in a Madrid jail. Puigdemont's party unexpectedly won the most seats among the main separatist parties in December, even though Puigdemont has not made clear whether he plans to return from Belgium. The Spanish leader has also described as "absurd" the idea that Puigdemont could lead Catalonia from overseas.
Mas was Catalan president between 2010 and 2016 before stepping aside, handpicking Carles Puigdemont as his successor.
In order to guarantee a separatist majority in a parliamentary vote this month, Junqueras and the other jailed separatists are expected to ask for special permission from Spain's judiciary to travel to Barcelona for one day to cast their votes.
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