"The appalling attacks on Aleppo have shaken all of us, and the violence and the attacks we have seen, also on an aid convoy, is morally totally unacceptable and is a blatant violation of international law," Stoltenberg told a news conference in Bratislava.
Stoltenberg did not identify the Syrian regime or its ally Moscow as being behind the pounding of the city by warplanes in which dozens of civilians including children have died, or a deadly attack on an aid convoy in Aleppo province last week.
But his comments came after Western powers slammed Russia over the violence with the United States accusing Moscow of "barbarism" and Britain and France alleging war crimes. Russia called that rhetoric "unacceptable".
Speaking after meeting EU defence ministers in the Slovakian capital, Stoltenberg said the ongoing violence "underlines the importance of finding a diplomatic and peaceful solution to the crisis in Syria".
"I join the international calls on Russia to show credible efforts to restore the cessation of hostilities, to allow humanitarian aid into Aleppo and to create the conditions necessary for UN-led transition talks to resume," he said.
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