Finance Minister P.Chidambaram and Maharashtra Navnirman Sena (MNS) chief Raj Thackeray cast their votes in Sivaganga District in Tamil Nadu and in Mumbai respectively on Thursday.
Speaking to media after exercising his franchise, a confident Chidambaram said: "I and my friends fully believe that we (the ruling Congress Party) will win these elections. The results of Tamil Nadu elections will be against projections."
"The Election Commission's role has been good, but there are orders which are very new and unheard of, and we have been criticising them," he added.
In Mumbai, Thackeray and his wife Sharmila Thackeray cast their votes.
The country is now over halfway through its nine-phased voting for a new parliament, with the Congress Party reported to be struggling to hold its ground against the Bharatiya Janata Party (BJP).
Polling for the sixth phase of Lok Sabha elections began early on Thursday morning in 117 constituencies spread over 11 states and one union territory.
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These are - all 39 seats in Tamil Nadu, 19 in Maharashtra, 12 in Uttar Pradesh, 10 in Madhya Pradesh, seven each in Bihar and Chhattisgarh, six each in Assam and West Bengal, five in Rajasthan, four in Jharkhand and one each in Jammu and Kashmir and Union Territory of Puducherry.
Voting commenced amid tight security at 7 a.m., and will end at 6 p.m.
In Uttar Pradesh, 167 candidates are in the fray for 12 seats. Chief Electoral Officer Umesh Sinha said 504 polling centres will be under direct observation through Web casting.