[1] Midcontinental surface aerosols have been measured at a small, minimally polluted city in summer and winter and on a nearby remote mountain in summer. Aerosol scattering, absorption, size distribution, and composition were measured using a three‐wavelength nephelometer, an aethalometer, a passive cavity aerosol spectrometer, a scanning mobility particle sizer, an Aerodyne quadrupole aerosol mass spectrometer, and conventional filter systems. Size‐dependent, time‐dependent, and averaged refractive indices are estimated from the aerosol composition measurements and then used to calculate time‐dependent aerosol scattering. The calculated scattering values show differences that are generally less than 5% on average for all three refractive indices, suggesting that the average refractive index is adequate for scattering estimations from time‐ or size‐dependent aerosol measurements. The calculated scattering (backscattering) at 550 nm ranges from 2% less to 23% greater (11–22% smaller) than that measured. These differences decrease at 450 nm and increase at 700 nm and significantly exceed these values if optical size distribution measurements are not corrected for an appropriate index of refraction. Optimal agreement between calculated and measured scattering is achieved on 4 of the 6 days investigated in detail, if the real refractive index of the aerosol organic species ranges from 1.45 ± 0.02 at 450 nm to 1.62 ± 0.05 at 700 nm. Single‐scatter albedos are also calculated and found to be in good agreement with those derived from the experimental observations, ranging from 0.79 to 0.87 in the city and constant, near 0.95, on the mountain top.