Pul, 47, was found hanging from a ceiling fan at his official residence. Incumbent Deputy Chief Minister Chowna Mein confirmed to IANS that Pul had committed suicide.
"We have also recovered a suicide note from the room where the former Chief Minister committed suicide. I am not in a position to divulge much at this moment," said a senior police official.
Hundreds of people, including supporters of Pul, took to the streets as news of the suicide went viral and shouted slogans against the present government led by Chief Minister Pema Khandu.
The agitated crowd gathered in front of the Chief Minister's residence and destroyed a coffin brought for Pul.
The demonstrators defied the security forces guarding Chowna Mein's house and entered and vandalized it. They also destroyed some parked vehicles.
Some of them demanded a probe by the Central Bureau of Investigation (CBI) to find out what forced Pul to kill himself and demanded the resignation of the Khandu government.
Pul was widely admired for his compassionate approach towards the needy. He was known for high probity in public life and honest politics.
After becoming the Chief Minister, Pul began holding 'Janata Darbar' every Saturday in different parts of the state to interact with the people.
He also allowed his helicopter to carry critically ill patients to Itanagar and to other places in the country for treatment.
Khandu called an emergency cabinet meeting and has announced a three-day mourning.
"The cabinet is shocked and shattered that our senior colleague and a seasoned leader took this extreme step," an official statement said.
In a message to Pul's wife, Khandu said: "It pains my heart to write to you at this moment of extreme grief. I humbly endure to share with you the saddest times of your life though I know that it would be hard to do so."
Although Khandu became the Chief Minister on July 16, Pul was yet to vacate the Chief Minister's residence as his house was being renovated.
A Congress leader, Pul took office on February 19, unseating then Congress Chief Minister Nabam Tuki.
Later, Pul and his supporters joined the People's Party of Arunachal (PPA), a regional outfit.
After the Supreme Court reinstated the Tuki government, Pul and his supporters returned to the Congress and supported Khandu to become the Chief Minister.
Congress MP Ninong Ering said he was shocked by Pul's suicide.
"Maybe loneliness crept into him. When your mind is empty, it is a devil's workshop," he said.
Prime Minister Narendra Modi condoled Pul's death.
"My thoughts are with the family and supporters of Kalikho Pulji on his sad demise. His service to Arunachal Pradesh will be remembered," he said.
Congress President Sonia Gandhi expressed shock over his death.
Extending her condolences to the family of Pul, Gandhi said: "I pray for the peace of the departed soul."
Congress Vice President Rahul Gandhi said he was "shocked and deeply saddened over the untimely demise of Kalikho Pulji. My heart goes out to his family".
Jitendra Singh, the Minister of State for Development for Northeastern Region, added: "Pul had a promising career that has been cut short."
Communist leader D. Raja called the suicide "shocking" and said it was for the central government to find out what had happened.
Congress MP Gaurav Gogoi, son of former Assam Chief Minister Tarun Gogoi, said: "We are really saddened. He was just 47 years old. We pray for Pul's family."
Pul, who represents Hyuliang constituency in eastern Arunachal Pradesh, had served in various capacities in Arunachal Pradesh including as Finance, Power and Tribal Affairs Minister.
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