Voters queued early in 89 constituencies across nine states and territories in the latest leg of staggered voting in the world's biggest election which ends with results announced on May 16.
Modi voted in the city of Ahmedabad in his home state of Gujarat before taking a "selfie" of his inked finger and flashing his party's symbol of the lotus flower to cheering crowds.
"After analysing the election process and the voter's mind until now, I can say that this time nothing can save the mother-son government... a strong government will come to power," said Modi dressed in all white.
"All citizens have to take part in the festival and make the democracy stronger," he added.
The Congress party, headed by Sonia Gandhi and her son Rahul, is widely expected to lose to Modi's resurgent opposition Bharatiya Janata Party (BJP) after a decade in power.
With the Congress campaign flailing with just over two weeks to go, another Gandhi, Rahul's sister Priyanka, has stepped up to lead a fightback by India's most famed political dynasty.
Priyanka this week called the battle against Modi and the BJP a "fight for the heart" of Hindu-majority but constitutionally secular India as the campaign grows increasingly bitter.
Modi is seen as a deeply polarising figure due to his Hindu nationalist rhetoric and failure to swiftly curb deadly 2002 anti-Muslim riots that swept Gujarat during his early years as chief minister of the prosperous western state.
About 140 million people were eligible to vote on Wednesday including in Modi's Gujarat and the battleground states of Bihar and Uttar Pradesh which alone sends 80 lawmakers to India's 543-member parliament.
Security was tight in Srinagar, the main city of disputed Indian Kashmir, where separatist leaders have called for a poll boycott and militants have threatened violence against voters who cast their ballots.
Hundreds of police and paramilitaries patrolled the streets of Srinagar which were mostly deserted except for a handful of voters.
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Sir No doubt Modi will creat history God must help him to surpass 272 seats.India urgently requirs a Hardcore dictator now lets hope he will overcome all hurdles-----
Selfie!!! Lolzz...
Pakistanis should not buy into the media's demonisation of Modi. In fact a strong leader in India is more likely to work towards resolving outstanding issues with Pakistan. As to muslims in India, they are edgy because of the Modi-fear the Congress-paid media have been spreading, but Modi's government will be a blessing in disguise for them for they will finally understand what being equal citizens truly means. Till now they have only been treated as a vote bank by the Congress and other so called secular parties. So rest easy and hope for a Modi win. His good governance will force even Pakistani politicians to focus on working for their people.
Ohoo jiyo mere laal!