This paper evaluates the feasibility of a method using a single hand-held infrared (IR) thermometer and a mini tower of wet and dry paper towels to psychometrically obtain surface layer temperature and moisture gradients and fluxes. Sling Psychrometers have long been standard measuring devices for quantifying the thermodynamics of near-surface atmospheric gas–vapor mixtures, specifically moisture parameters. However, these devices are generally only used to measure temperature and humidity at one near-surface level. Multiple self-aspirating psychrometers can be used in a vertical configuration to measure temperature and moisture gradients and fluxes in the first 1–2 m of the surface layer. This study explores a way to make multiple vertical psychrometric measurements with a single non-contact IR temperature sensor rather than using two in situ thermometers at each level. The surface layer dry- and wet-bulb temperatures obtained using an IR Thermometer are compared to Kestrel 4000 Weather Meter and Bacharach Sling Psychrometer measurements under various atmospheric conditions and surface types to test the viability of the method. To evaluate the results obtained using this new approach, standard meteorological surface data are collected during each experiment, and moisture parameters are derived via psychrometric equations. The results indicate that, not only is the method possible and practical, but they suggest that the IR Thermometer method may provide more surface layer temperature and moisture gradient and flux sensitivity than other single instrument methods.