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The influence of the photothermal laser source beam size on the measurement sensitivity of layered systems using photothermal radiometry (PTR) is presented. Based on an appropriate theoretical model, widely different behaviors of the photothermal amplitude and phase in terms of combinations of thermophysical properties (i.e., thermal conductivity and thermal diffusivity) between a thin coating and the substrate are observed. The beam size effect on PTR measurement sensitivity is theoretically examined and experimentally demonstrated using a carbonitrided C1018 steel sample. The experimental results of using a variable size laser beam for the carbonitrided C1018 sample validate the theoretical prediction, in which an expanded beam exhibits a much larger magnitude change in both amplitude and phase as a function of frequency than measurements with a focused beam. The fitted thermal conductivity and thermal diffusivity based on the assumed industrially relevant range of effective hardness case depth gives the approximate range of the change in thermal conductivity and thermal diffusivity of C1018 steels after the carbonitriding process.