Dozens are feared dead after the school in Bilohorivka in the Luhansk region of eastern Ukraine was bombed and caught fire on Saturday.
The Foreign Secretary said she was "horrified" and added Vladimir Putin's regime in Moscow would be held to account.
Around 90 people were thought to have been sheltering at the school but just 30 have been rescued.
Ms Truss tweeted: "Horrified by Russia's latest attack on a school in Luhansk, resulting in the deaths of innocent people sheltering from Russian bombardment."
She said the deliberate targeting of civilians and infrastructure "amounts to war crimes” and “we will ensure Putin's regime is held accountable".
Her comments came as G7 leaders, including Boris Johnson and Joe Biden, prepared for talks with Ukraine's president Volodymyr Zelensky.
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