After retiring from the army with the rank of major in 1960, he began lecturing in mathematics at the Belfast College of Technology and became politically active, initially as an election agent for Gerry Fitt.
He later joined forces with Ian Paisley, and became a leader of the Ulster Protestant Volunteers and the Loyal Citizens of Ulster. He and Paisley were imprisoned for leading the loyalist group that disrupted an NICRA march in Armagh in November 1968. The following January, Bunting also led the loyalist protesters against the People’s Democracy march from Belfast to Derry. Ronald Bunting was the father of republican activist Ronnie Bunting.