Singh, 80, filed his nomination papers before Assam Assembly's Principal Secretary G P Das, who is also the returning officer for the polls.
During his three-hour visit here, he filed the nomination papers amidst protests from media persons outside the Assembly gate as they were prevented from entering the premises for covering the event.
Prior to filing his nomination, the Prime Minister presided over the Congress Legislature Party's meeting in the the Assembly.
Assam Chief Minister Tarun Gogoi, Union Minister of State for Tribal Affairs Ranee Narah, Assam Pradesh Congress President Bhubaneswar Kalita along with several ministers were present on the occasion.
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The Prime Minister in a brief interaction with the media expressed his gratitude to the people of Assam for making it possible for him to file nomination for the Rajya Sabha for the fifth time since 1991.
"Assam has done a great service to me by sending me to the Rajya Sabha. I cannot be grateful enough to the people of Assam," he said.
Singh's term as Member of Parliament expires on June 14 with the Election Commission announcing the polls for two Rajya Sabha seats from Assam on May 30, the second seat being held by AGP MP Kumar Deepak Das.
The notification for the polls was issued on May 13 and the last date for filing of nominations is May 20.