Police said Mahendra Pradhan, a council member of the Gorkha Territorial Administration and Narayan Pradhan, president of the GJM Darjeeling Town Committee, were arrested in connection with old cases.
Mahendra Pradhan was picked up from his home at Sonada, near Darjeeling during the day in a drive by the police headed by the SP Kunal Agarwal, while Narayan Pradhan was taken into custody in the early hours from the town.
Mahendra Pradhan is the third GTA member to be arrested. The two others were Atin Thapa and Praksh Gurung.
West Bengal Chief Minister Mamata Banerjee,during the day, declared the indefinite bandh in Darjeeling to demand Gorkhaland as illegal and gave a 72-hour deadline for its withdrawal.
A defiant GJM has said it will call a 'janta curfew' and its members held protest gatherings at varous places in the hills and shouted anti-government slogans.