Behera, who resumed at his overnight score of 143, faced 453 balls and struck 19 boundaries and four sixes during his marathon knock.
But another overnight centurion Ranjit Singh (112) could added just three runs before being dismissed by Harshal Patel.
But Behera and Halhadar Das (93) shared 157 runs for the sixth to take Odisha forward.
Das scored his runs off 155 balls with the help of nine boundaries and three hits over the fence.
Patel (2/94) Jayant Yadav (2/164) picked up two wickets each for Haryana.
In reply, Haryana finished the day on 38 for no loss in 15 overs.
Rahul Dewan was batting on 26, while giving him company was Nitin Saini on 12.
Brief Scores:
Odisha: 529 for six decl in 163 overs (Natraj Behera 255 not out, Ranjit Singh 112, Halhadar Das 93; Harshal Patel 2/94).
Haryana: 38 for no loss in 15 overs (Rahul Dewan 26 not out, Nitin Saini 12 not out).
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