Raina's score is the third highest innings in a Twenty20 international and included nine fours and five sixes as he peppered the ball around the field with superb timing and placement.
The 23-year-old enjoyed a big slice of luck in the fifth over, though, when he was caught off a no-ball from Albie Morkel.
Yuvraj Singh's 37 contributed to a key 88-run partnership with Raina, who brought up his ton with a massive six over mid-wicket in the final over before he was caught off the next ball from Albie Morkel.
South Africa found themselves struggling to keep up with the run rate. Jacques Kallis, opening the batting, made a smart 73 off 54 balls but with the tempo too slow, a lot of work was left to the middle order.
AB de Villiers made a great attempt to snatch victory, hitting three sixes in his 31 off 15 balls before he was caught in the deep.
India won their opening group C match against Afghanistan on Saturday leaving South Africa now needing to beat the tournament's minnows to make sure of advancing.
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