Staffan de Mistura told reporters in Geneva that there were "indications that after Daraya we may have other Darayas," adding that "there is clearly a strategy at the moment to move from Daraya" to other besieged areas "in a similar pattern".
Long held by opposition forces, Daraya near Damascus was ravaged by constant army bombardment, and just one aid convoy reached the town since it came under siege in late 2012 - arriving in June this year.
Hundreds of fighters and their families were bused north into rebel-held territory in Idlib province, with other civilians transferred to government territory near Damascus for resettlement.
The Syrian army has said it is in complete control of the town, from where roughly 8,000 civilians were still due to be evacuated.
De Mistura warned there were "indications that after Daraya we may have other Darayas," pointing to worrying signs around the besieged towns of Waer and Moadamiyat al-Sham.
"If Daraya was a shock, Al Waer is 75,000 people," he pointed out.
He insisted that the devastating sieges in Syria could not be "broken by a population giving up after starvation and after bombing".
"A siege is lifted by humanitarian access and freedom of movement in and out by the civilian population," he said.
"We all failed the people of Daraya," he said, adding that the UN was receiving "urgent pleas" from besieged communities in Waer, Moadamiyat al-Sham, Madaya, Fua and Kefraya.
"They all fear for their future, and we need to break the sieges," he said.
"The Syrian regime, along with its Russian and Iranian allies, is relentlessly pursuing a malicious plan to orchestrate extensive demographic shifts across Syria," HNC head Riad Hijab said in a statement late yesterday.
Egeland meanwhile said that humanitarian aid reached just three besieged areas last month, with two convoys reaching Waer, one reaching Harasta, and continued air-drops over Deir Ezzor, which is held by the Islamic State group.
"September must be better," he said, adding that the humanitarian taskforce had yet to receive a reply to its request to access 1.2 million people in besieged and hard-to-reach areas with aid this month.
More than 290,000 people have been killed in Syria since the conflict began in March 2011.
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