Record turnout is expected in a vote pitting leaders of the wealthy northeastern region's separatist movement against parties that want to remain in Spain.
Will voters again hand victory to pro-independence parties that tried to break Catalonia from Spain, one of whose candidates is in jail and the other in self-imposed exile in Belgium?
Or will they lose the absolute parliamentary majority of 72 seats they won in 2015?
While the independence question is far from new, it was the referendum on October 1 -- and a heavy police crackdown on voters -- that focused the world's attention on the region.
Some 5.5 million people are registered to vote in Thursday's election which is likely to see seven parties winning mandates in the 135-seat regional parliament.
Even before polling stations opened in Barcelona, people had formed long queues to cast their ballots.
"We had to vote today, we couldn't have stayed home," he said, adding that he was voting for the pro-unity camp.
The vote is widely seen as a plebiscite on the independence question in Catalonia, whose autonomy Spain stripped in an unprecedented move after a failed independence declaration on October 27.
Crucially, however, even if the pro-independence camp wins, it is not expected to attempt another breakaway from Spain but rather try to enter into negotiations with Madrid.
In the staunchly pro-independence town of Vic, the sun shone feebly on a small line of voters waiting in the freezing cold outside a day centre for the elderly, their polling station.
Posters advocating independence were plastered all over the nearby walls, one of which had a picture of someone's hands tied behind their back, which read: "Help Catalonia".
Following the controversial October referendum, which went ahead despite a ban by Madrid, the crisis came to a head later that month when the regional parliament declared unilateral independence.
The move infuriated the Spanish government but also rattled a Europe still reeling from Britain's decision to leave.
The secession bid was short-lived, though, as Madrid sacked Catalonia's government, dissolved its parliament and called snap elections.
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