In this paper we report a combined calorimetric and inelastic neutron scattering (INS) study of hydrated γ-Al2O3 (γ-alumina) nanoparticles. These complementary techniques have enabled a comprehensive evaluation of the thermodynamic properties of this technological and industrially important metal oxide to be achieved. The isobaric heat capacity (C(p)) data presented herein provide further critical insights into the much-debated chemical composition of γ-alumina nanoparticles. Furthermore, the isochoric heat capacity (C(v)) of the surface water, which is so essential to the stability of all metal-oxides at the nanoscale, has been extracted from the high-resolution INS data and differs significantly from that of ice-Ih due to the dominating influence of strong surface-water interactions. This study also encompassed the analysis of four γ-alumina samples with differing pore diameters [4.5 (1), 13.8 (2), 17.9 (3), and 27.2 nm (4)], and the results obtained allow us to unambiguously conclude that the water content and pore size have no influence on the thermodynamic behaviour of hydrated γ-alumina nanoparticles.