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Patole, elected from Bhandara-Gondiya, said he submitted his resignation to Lok Sabha Speaker Sumitra Mahajan's office and also to the Bharatiya Janata Party leadership. He said he was "deeply anguished and felt let down by the party".
His brief resignation letter addressed to Mahajan read: "Respected Madam, I hereby tender my resignation of my seat in the House with effect from today i.e. 08/12/17."
The development is seen as a blow to the BJP, coming a day ahead of the first round of the Gujarat Assembly polls on Saturday.
"The objectives with which I had joined the (BJP) party have been belied, but now (post-quitting) I am free of the turmoil in my mind," Patole told the media shortly after submitting his resignation letter to the Lok Sabha Secretariat.
He said he had not made up his mind on which party to join but would consider throwing his lot with "some like-minded" political outfit.
In Mumbai, Maharashtra Chief Minister Devendra Fadnavis said he was yet to get full details on the matter and would "comment at the appropriate time".
Patole said that after taking power, the BJP had forgotten all its promises and assurances it made to the electorate.
Patole, the first BJP to quit the party and the Lok Sabha after Modi took office in 2014, created a sensation when he told a public function that the Prime Minister does not like to be questioned and criticized.
He also alleged that all central ministers "were always in a state of fear" and that he was "on the hit list but I am not afraid of anyone".
Earlier this week, Patole shared limelight with senior BJP leader Yashwant Sinha who led a farmers' agitation in Akola for three days, which ended on Wednesday with Fadnavis agreeing to concede all seven major demands.
Patole had earlier labelled the Modi government "deaf and blind" and accused it of allegedly favouring top industrialists and showing little concern for ordinary people including farmers.
(This story has not been edited by Business Standard staff and is auto-generated from a syndicated feed.)