The 77-year-old spent a week in Aleppo, where he came under sniper fire as he tried to take pictures of the conflict.
McCullin told BBC Radio 4's Front Row he "hadn't seen any real evidence of what's been going on" in Syria, so he decided to take one final assignment.
His aim, he added, was to show the human toll of the fighting.
The photos, published in The Times newspaper on Thursday, focus on families displaced by what he described as "constant heavy shelling".
One picture, replicated at the top of this page, depicts a group of children hunting for water supplies on the streets of the war-ravaged city.
"We don't need any more scenes of snipers and rebels firing over brick walls," he told the BBC. "What we really need is the human interest side of this story."
"The children play on the streets here as if it's Guy Fawkes night, with all these explosions going on around them.
"The great tragedy is that, if only the people in Russia knew that their taxes were going on making these dreadful weapons that were killing innocent people here, they might think twice about their leadership."
'Ghastly scenes'McCullin has braved war zones in Vietnam, Lebanon and Cyprus during his long and industrious career, spending more than 18 of his 50 years as a photographer on the front line.
He was wounded by fragments from a mortar shell in Cambodia, temporarily blinded by CS gas during a riot in Derry, and arrested by Idi Amin's henchmen in Uganda.
After coming back from Iraq in 2003, he announced his intention to retire from war photography and settle down in Somerset.
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