In a series of systematic studies, we have investigated the molecular motion in crystals of the glycine polymorphs and determined their thermodynamic functions from an analysis of multitemperature atomic displacement parameters (ADPs) combined with ONIOM calculation on 15-molecule clusters. The studies are aimed at providing insight into the factors governing the relative stabilities of the α-, β-, and γ-polymorphs. This Article, the last in the series, focuses on the most stable polymorph, γ-glycine. Multitemperature diffraction data of the γ-glycine polymorph have been collected to 0.5 Å resolution between 10 and 300 K at two synchrotron beamlines, KEK Photon Factory and ID11 of the ESRF. The ADPs of γ-glycine from these sources differ significantly, as previously observed also for the other two polymorphs. A simple model of rigid body motion explains the ADPs from KEK and their temperature dependence. It provides lattice vibration frequencies that are in line with those from Raman spectroscopy. Together with the internal vibration frequencies from an ONIOM calculation, the thermodynamic functions are estimated using the Einstein, Debye, and Nernst–Lindemann models of heat capacity. The relative stabilities of the three polymorphs of glycine are discussed on the basis of the contributions to their free energies as obtained in this work and from various experimental and theoretical studies. The comparison shows that the free-energy differences are determined primarily by differences in lattice and zero-point vibrational energies.