Worldwide use of hydrofluorocarbons (HFCs) is currently being regulated and phased out because of high global warming potentials (GWPs). Separation techniques for recycling refrigerants are needed so that HFCs can be dealt with responsibly. Many HFCs currently in use are azeotropic or near-azeotropic refrigerant blends and must be separated so that the components can be recycled and repurposed effectively. One such refrigerant is R-410A, which is a near-azeotropic 50/50 wt % mixture of pentafluoroethane (HFC-125) and difluoromethane (HFC-32). This study examined the use of the LTA zeolites for separating HFC-32 from HFC-125. Pure gas isotherms were measured using a XEMIS gravimetric microbalance with zeolites 3A, 4A, and 5A. Reversible sorption was observed for HFC-32 with zeolites 4A and 5A, whereas irreversible sorption was observed for HFC-125 with zeolite 5A. Negligible sorption was observed for HFC-125 with zeolites 3A and 4A, and although sorption of HFC-32 with zeolite 3A was observed, the process was slow, making the sorbent not commercially viable. The enthalpy of adsorption was predicted using the vapor adsorption equilibrium (VAE) analogue of the Clausius-Clapeyron equation and measured using a calorimeter for HFC-125 and HFC-32 with zeolite 5A and for HFC-32 with zeolite 4A. Molecular-level interactions between the LTA zeolites and HFCs were discussed and used to interpret pure gas isotherms and enthalpy of adsorption results. Overall, zeolites 4A and 5A were found to be good candidates for kinetically and thermodynamically separating R-410A, respectively.