The left-hander hit 33 boundaries and three sixes for North Zone before being dismissed on the second day of the four-day Duleep Trophy semi-final against Central Zone in Hyderabad.
Yuvraj, 30, who was judged man of the tournament in India's 50-over World Cup triumph last year, was treated for a rare germ-cell cancer between his lungs in the United States earlier this year.
He returned after energy-sapping chemotherapy treatment in April and by August had been fast-tracked into the Indian team for the recent World Twenty20 in Sri Lanka.
Yuvraj ended the tournament with 66 runs in four innings and claimed eight wickets in five matches, the second highest among Indian bowlers after seamer Lakshmipathy Balaji's nine wickets.
India, the 2007 champions, won four of their five matches but failed to reach the semi-finals of the event eventually won by the West Indies.
Yuvraj's double-century is certain to put him in line for a recall when the four-Test series against England starts in Ahmedabad on November 15.
He has not played Test cricket since November last year when he turned out for two matches against the touring West Indies.
Yuvraj has played 37 Tests since his international debut in 2000, scoring 1,775 runs at an average of 34.80 with three centuries. He has also claimed nine Test wickets with his left-arm spin.