"The Army of Conquest on Saturday took control of the armament school, where there is a large amount of ammunitions, and a large part of the artillery school", the Syrian Observatory for Human Rights said.
The coalition "is about to cut off, by gunfire, the supply route into government-controlled districts" of the city, Observatory head Rami Abdel Rahman said.
The road, which passes through a southwestern suburb of Aleppo city called Ramussa, is the last open route into Aleppo city.
The former Al-Nusra Front - renamed Jabhat Fateh al-Sham after breaking from Al-Qaeda - today announced having captured the two military academies and a third military position.
State television, meanwhile, reported fighting in the three locations.
"The regime forces are in a very difficult position despite Russian air support," Abdel Rahman said.
Once Syria's economic powerhouse, Aleppo has been roughly divided into a rebel-held east and regime-controlled west since 2012.
The jihadist and rebel advance comes three weeks after regime forces backed by Russian air strikes besieged the city's opposition-held districts, raising fears of a humanitarian crisis there.
More than 280,000 people have been killed since the conflict started with the brutal repression of anti-government protests in 2011.
Russia launched air strikes in Syria in support of the regime in September last year.
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