The winning candidate in the Election of President of India should fulfill the requirement mentioned in option 4 - they must secure more than fifty percent and majority of the total votes polled. This means that in order to be declared as the winner, the candidate must obtain both a majority of the votes and more than half of the total number of votes cast in the election.

Option 1 states that the winning candidate should secure the majority number of votes polled. While this may seem similar to option 4, it fails to consider the requirement of also securing more than fifty percent of the total votes polled.

Option 2 states that the winning candidate should secure sixty-six percent of votes polled. This is incorrect as it does not account for the requirement of obtaining a majority of votes.

Option 3 states that the winning candidate should secure fifty percent of votes polled. This is also incorrect as it does not consider the need for a majority of votes.

Therefore, option 4 is the correct answer.