The viscosity and surface tension of binary mixtures of glycerol (1) + N-methyl-2-pyrrolidone (2) at T = 293, 298, 303, 308, 313, 318, and 323 K and at atmospheric pressure are reported. The Jouyban–Acree model was used for mathematical correlation of measured data. The average percentage deviation was used as an accuracy criterion. Derived properties from measured thermophysical properties, including deviations in viscosity and surface tension; the enthalpy, entropy and Gibbs energy of flow activation; standard enthalpy and entropy of surface formation data were reported.