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We evaluated the effects of hydration heat inhibitors on the early hydration heat release process of cement and its main mineral components. We used a microcalorimetric method to determine the effects of various proportions and properties of hydration heat inhibitors on the hydration of portland cement, tricalcium silicate, and tricalcium aluminate: concentration (C) = 40% m/m hydroxydiphosphonic acid (HEDP) (1-hydroxyethylidene-1,1-diphosphonic acid) and C = 40% m/m diethylene triamine pentonyphosphonic acid (DTPMPA) (diethylenetriaminepentamethylene phosphonic acid). We also analyzed and tested the heat release rate and cumulative heat release during the hydration of cement and its main mineral components. The hydration heat inhibitors decreased the heat release rate of cementitious materials by means of adsorption, chelation, precipitation, complex formation, and control of calcium hydroxide crystals. Among these materials, the hydration heat inhibitor had the most substantial effect on the composition of tricalcium silicate clinker, reducing the peak temperature at the initial stage of hydration and delaying its occurrence time. These results are pertinent to controlling and selecting the early hydrothermal release process of cement systems.