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Long-term confinement of nuclear waste is one of the main challenges faced by the nuclear industry. Fission products such as ⁹⁰Sr and ¹³⁷Cs, both β⁻ emitters known to induce serious health hazards, represent the largest fraction of nuclear waste. Cement is a good candidate to store them, provided it can resist the effects of irradiation over time. Here, we have investigated the effects of β⁻ decay on cement by performing electron irradiation experiments on different samples. We show that H₂ production in cement, the main effect of water radiolysis, depends strongly on composition and relative humidity. First-principles calculations indicate that the water-rich interlayer regions with Ca²⁺ ions act as electron traps that promote the formation of H₂. They also show that holes localize in water-rich regions in low Ca content samples and are then able to participate in H₂ production. This work provides new understanding …