Experimental relationships between the mass concentration of suspended particulate matter and the optical density of particulates collected on paper tape have been determined for the atmospheric aerosol and for aerosols of constant optical properties. Simultaneous samples were obtained on membrane filters (for gravimetric analysis) and on Whatman No. 4 paper tape (for optical evaluation). Sampling procedures were adopted which ensured that the efficiency of sampling was the same in both cases. Consistent relationships between mass concentrations of suspended particulate matter and optical density expressed in terms of per cent transmittance or per cent reflectance were found for dispersions of coal, limestone, fly ash, and a coal-limestone mixture. For atmospheric aerosol samples collected on the roof of the Graduate School of Public Health, University of Pittsburgh, the relationship between mass concentration and per cent transmittance or per cent reflectance was found to be linear over the range of values observed. The correlation coefficients were −0.93 (for concentration versus per cent transmittance) and −0.89 (for concentration versus per cent reflectance).