AbstractLow‐temperature heat capacities of gramine (C11H14N2) were measured by a precision automated adiabatic calorimeter over the temperature range from 78 to 401 K. A polynomial equation of heat capacities as a function of temperature was fitted by least squares method. Based on the fitted polynomial, the smoothed heat capacities and thermodynamic functions of the compound relative to the standard reference temperature 298.15 K were calculated and tabulated at 5 K intervals. The constant‐volume energy of combustion of the compound at T=298.15 K was measured by a precision oxygen‐bomb combustion calorimeter as ΔcU=−(35336.7±13.9) J·g−1. The standard molar enthalpy of combustion of the compound was determined to be ΔcHm0=−(6163.2±2.4) kJ·mol−1, according to the definition of combustion enthalpy. Finally, the standard molar enthalpy of formation of the compound was calculated to be Δ;cHm0=−(166.2±2.8) kJ·mol−1 in accordance with Hess law.