Gurung had then held a meeting with former army personnel and officers from the hills and requested them to take charge of selection, recruitment and training of the youths.
The police fired teargas shells and baton-charged the agitators.
At least 12 people have been injured in riots and arson attacks that have gripped the usually bustling area for more than a week and caused thousands of mostly Indian tourists to pack their bags and flee.
"We think the police and security personnel should be immediately removed from Darjeeling to create conducive environment for talks". They are both martyrs.
Mamata Banerjee condemned the vandalism by the GJM and alleged "deep-rooted conspiracy".
"The final battle is on".
Police claimed to have seized bows and arrows, knives, axes, explosives and a large quantity of cash from Gurung's house.
However, police have claimed that the deaths were not due to police firing. The report further added that GJM supporters had been killed in police firing after their women's wing - Nari Morcha - organised a rally in Singmari.
The situation remains tense as the indefinite bandh called by the Gorkha Janmukti Morcha (GJM) has entered the sixth day today. Tamang, who belongs to IRS's 2nd Battalion, has been shifted to a private nursing home in Siliguri, the police said.More news: Kohli hints at same playing XI in CT17 Final against Pakistan
More news: Virat Kohli tells team to stay off social media. Here's why!
More news: Britain to hold special two-year parliament session to tackle Brexit
Referring to the CBI naming senior GJM leaders in the Akhil Bharatiya Gorkha League leader Madan Tamang's murder, Banerjee said its chief Bimal Gurung was a "corrupt leader" trying to sell off the hills and hampering the development work taken up by the state government there.
"Whatever is happening is a deep rooted conspiracy", Banarjee told reporters. So many bombs and arms can not be gathered in a day.
Darjeeling has been on the boil for the past ten days and indefinite shutdown is on by GJM in support of its separate Gorkhaland demand.
She also voiced her suspicion that a foreign country could also be backing the current unrest in the hills. "We have got information that the GJM have connections with underground insurgent groups in the northeast". All security forces deployed in Darjeeling have been put on high alert and flag marches are being conducted in various parts of the hill city.
Meanwhile, West Bengal chief minister Mamata Banerjee, who was felicitating journalists Bartaman Bhavan by naming roads and community halls after them yesterday said, "Banglake bhaag hote debo na (I will not let Bengal be divided)".
The slogan-shouting protesters did not relent and started throwing petrol bombs, stones and bottles at the police, he said. The anti-Bengla agitation has now metamorphosed into a separate statehood movement, with GJM going back to its pre-2012 position. The protests had started against "imposition" of Bengali language in schools.
Tamang also claimed police arrested Vikram Rai, son of GJM MLA Amar Rai. Vikram is the in-charge of the GJM's media cell.
A police team, led by Darjeeling SP Akhilesh Chaturvedi, raided Gurung's office and house in Patlybas and recovered sophisticated cross bows, a huge cache of arrows, explosives, spades, axe, sickle and cash.