The government advance angered the opposition, further undermining prospects for peace talks underway in Geneva. The two villages, Nubl and Zahra, are located in the middle of opposition territory.
They have been blockaded by rebel groups for around three years, with the army occasionally airdropping food and other assistance.
Their capture would mark a major victory for government forces, which have made significant advances in Aleppo province in the past few days, severing a key supply route linking rebels in Aleppo city to the Turkish border.
The Aleppo advances cast a further shadow over indirect peace talks in Geneva.
Basma Kodmani, a member of the opposition's negotiating team, described the offensive as a "horrible development," saying it sends the message that "there is nothing to negotiate. Just go home."
"We're not going home," she said in an interview with The Associated Press.
The Britain-based Syrian Observatory for Human Rights, an opposition group that monitors the conflict through activists on the ground, said the Syrian army was one kilometer away from the two villages.
Meanwhile, an aid convoy headed to a besieged rebel-held town near Damascus, but Syria's opposition said today that such deliveries are meaningless given the situation in Aleppo.
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