Variable-temperature fast field cycling NMR measurements are used to probe the surface dynamics of different liquids imbibed within a γ-alumina catalyst support material. The imbibed liquids were grouped as nonpolar, polar aprotic, and polar protic; the surface dynamics were found to depend strongly on the chemical properties of the adsorbate. For almost all liquids, a single relaxation environment was observed. However, for methanol, the relaxation behavior of the hydroxyl and methyl groups showed distinct temperature-and frequency-dependent behavior, demonstrating the occurrence of a functionality-specific relaxation process. The nuclear magnetic relaxation dispersion (NMRD) profiles of the protic functionalities were renormalized to a single NMRD profile, indicating a common relaxation process. Further insight was achieved by modeling the NMRD profiles. For nonpolar species, translational diffusion in the presence of paramagnetic impurities dominated the relaxation, and the solid−liquid interaction strength ranked as toluene > cyclohexane ≈ n-heptane. For polar aprotic liquids, the data were consistent with relaxation being dominated by an intermittent surface binding mechanism, and the adsorbates ranked as methanol > dimethyl sulfoxide (DMSO) > tetrahydrofuran (THF). Finally, for polar protic liquids, the relaxation was controlled by a chemical exchange process that resulted in a surface diffusion of the labile 1 H species in the presence of paramagnetic impurities.