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Evidence from rescue workers "strongly suggests" Syrian government forces used toxic chemicals during barrel bomb attacks in Idlib, according to Human Rights Watch.
The New York-based group says eyewitnesses reported multiple attacks between 16 March and 31 March in the north west of the country.
Six civilians, including three children, died in one of the attacks, according to HRW. At least 206 people were affected in total.
The group investigated six attacks in which Syrian government helicopters dropped barrel bombs containing gas canisters.
Eyewitness accounts, photographs and video footage from three of the attacks indicate the use of a chemical agent, possibly chlorine.
A canister found in the remnants of a barrel bomb on 24 March (Pic: HRW)
HRW is continuing to probe the other three attacks.
Nadim Houry from HRW said: "Syrian authorities appear once again to have shown complete disregard for human suffering by violating the global prohibition against chemical warfare.
"The UN Security Council and countries that are members of the Chemical Weapons Convention need to respond strongly."
The most conclusive evidence came from an attack on 16 March in the village of Sarmin.
"The children were foaming at the mouth, they were suffocating, then their hearts stopped," said Leith Fares, a rescue worker in Sarmin.
A Syrian security official denied the claims, saying the accusations were "lies the insurgents say when they incur losses".
The official told the AFP news agency: "If the army used chemical weapons or chlorine gas every time they say it did, those people would have been completely wiped out by now."
In March the UN Security Council adopted a resolution condemning the use of chlorine in Syria and threatening sanctions if the chemicals were used.
Syria was not forced to declare its stocks of chlorine under a 2013 agreement to dismantle its chemical arsenal as the substance is widely used for commercial and domestic purposes.
But the use of the gas for military purposes would be a breach of its undertakings under the Chemical Weapons Convention, which it signed as part of the deal.