Party treasurer and senior leader, R Masilamani resigned from his post and primary membership. Madurai Rural District Secretary, P Saravanan too tendered his resignation.
The development assumes significance as only yesterday Salem District Secretary Thamaraikannan and party women's wing secretary Kumari Vijayakumar quit the party to join DMK in the presence of party chief Karunanidhi.
Last week, Kancheepuram district secretary Palavakkam Somu too had switched allegiance to DMK.
"I am happy if their expectations get fulfilled now," he told reporters at nearby Mamallapuram.
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Saravanan did not, however, buy Vaiko's argument, whom he accused of taking unilateral decisions. "He has been taking unilateral decisions without consulting district secretaries, functionaries and workers," he said.
"Only two months back he told us that the we could fight polls alongside the DMK and he changed his stance soon after," he told PTI.
"He now says that the party will face polls by leading the five-party People's Welfare Front. This won't succeed and retaining deposits itself will not happen anywhere, leave alone winning," he said.
On September 15, Vaiko categorically stated at a party meet in Tirupur that his party would not forge an electoral pact with either AIADMK or DMK.
He had said that the party would face polls alongside CPI, CPI(M), and VCK and also try to rope in the MMK which are part of the People's Welfare Front.
The five party combine PWF was a recent initiative of these parties to "fight for the people's issues and anti-people central and state policies."
Though the duo have not disclosed their future moves, it is expected that they may join DMK following other colleagues who had quit just ahead of them.