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Herein, the radiolytic degradations of atrazine and cyanuric acid were performed via electron beam irradiation. The results demonstrated atrazine could be completely mineralized without any residue of cyanuric acid in aqueous solution. The degradation of atrazine followed the pseudo-first-order reaction kinetics. The studies in the presence of different radical scavengers (O2 and tert-butanol) indicated hydroxyl radicals were the main species for the decomposition of atrazine into cyanuric acid, while e−aq played vital role in the degradation of cyanuric acid. During the radiolysis processes of atrazine and cyanuric acid, some organic and inorganic intermediates were detected, implying dechlorination, dealkylation, and deamination occurred. On the basis of the effects of radicals and detected products, the potential radiolytic degradation pathways of atrazine via electron beam were proposed.