Raina made 123 off 154 balls, hitting 12 fours and four sixes in the process after Uttar Pradesh opted to bat at the Moti Bagh Stadium.
The visitors were placed at 291 for nine at stumps on the first day. Left-arm spinner Bhargav Bhatt (5/98) and off-break bowler Utkarsh Patel (4/74) were the wreckers in chief for Baroda. Former India player Mohammed Kaif contributed 39 and Parvinder Singh made 35.
Batting first, the visitors were off to a sedate start as openers Tanmay Srivastava (23) and Mukul Dagar (27) put on 52 runs for the first wicket.
Raina was involved in an 85-run stand for the third wicket with Kaif, before adding 110 runs for the fourth with Parvinder, who scored his runs off 77 balls while spending 226 minutes in the middle, with the left-hander preferring to take bulk of the strike.
At the close of play, Imtiaz Ahmed was batting on 3 with last-man R P Singh to come tomorrow.