An improved internal reflection infrared spectroscopy (ATR) technique (1) has been found to be effective for measuring the relative concentrations of polyester and polystyrene (resin) and calcium carbonate filler on sheet molding compound (SMC) surfaces. The technique has been used to determine the effect of molding conditions on the surface compositions of three commercial SMC materials. The surface compositions of two of the materials, of the same formulation but obtained from different sources, were the same and were unaffected by molding conditions. The surface of the third material (of a different formulation) was found to have substantially less resin than the first two materials. The surface composition of the third material varied with molding conditions, the greatest uniformity being obtained with high molding temperatures and pressures. This study has shown that the ATR technique is suitable for determining the relative surface compositions of SMC formulations. This method will be used to correlate the SMC surface composition to SMC properties, such as surface appearance, paintability, and adhesive bond durability.