Addressing an election rally here in Kamrup district, the prime minister said the Bharatiya Janata Party (BJP) and its allies wanted to form "a majority government" in the state.
"Some people are waiting to see a hung assembly in Assam. They want to remote control Assam from Delhi," he said, in an obvious reference to the state's ruling Congress party.
"So make sure that the BJP alliance gets an absolute majority."
Modi also accused the Congress of exploiting what he called was the Bangladeshi vote bank to stick to power.
"The people of Assam have supported the Congress wholeheartedly for 15 years. But the party has failed to reach beyond its Bangladeshi vote bank and dynastic politics, ruining the state," he thundered.
The prime minister said that fencing the winding India-Bangladesh border was his priority.
He said his government would take such steps that would not only stop infiltration from Bangladesh but ensure that all the illegal infiltrators living in Assam were sent back.
And in an obvious dig at the Congress, Modi wondered why Saudi Arabia's decision to confer the highest civilian award on him had upset some people in the state.
"I understand a certain country won't like India's relationship with some foreign country improving. But why a section of people here are having stomach ache? What kind of patriotism is this?"
Earlier, at another rally at Raha in Nagaon district, Modi said Assam Chief Minister Tarun Gogoi had stopped smiling after the heavy polling in the first phase of assembly elections on April 4.
And the Congress leadership cannot save the party from defeat in the polls, the second and final phase of which will be conducted on Monday, he said.
Modi arrived in Assam on Friday to campaign for the BJP. Polling for 61 constituencies will take place on Monday.
The prime minister first visited the Kamakhya temple in Assam's main city Guwahati.
"I thank the people of Assam for the unprecedented high percentage of voting in the first phase," Modi said, addressing the crowd at Raha in Hindi.
"You must have noticed that the Assam chief minister has stopped smiling after the first phase. He is now inviting Congress leaders from Delhi to save him.
"But how can they (Congress leaders) save Gogoiji when they could not even save Delhi?" he asked, referring to the 2014 Lok Sabha polls.
He said he had come to Assam to seek the people's support to bring about a change of government in the state.
Modi said he had not seen another state in India apart from Assam where he claimed the entire population lived below poverty line (BPL).
"There are states in India where there are 20 or 30 percent BPL population. But the Congress in Assam has turned the entire population of the state poor as BPL."
He said there should be a new government in the state.
A total of 65 constituencies in Assam saw a record 82.20 percent polling in the first phase on April 4.