The main aim of the work was complex experimental measurements of microphysical, chemical, and optical parameters of aerosol particles in the surface air layer and free atmosphere. From the measurement data, the entire set of aerosol optical parameters was retrieved, required for radiation calculations. Three measurement runs were carried out in 2013 within the experiment: in spring, when the aerosol generation maximum is observed, in summer (July), when the altitude of the atmospheric boundary layer is the highest, and in the late summer – early autumn, when the second nucleation period is recorded. The following instruments were used in the experiment: diffusion aerosol spectrometers (DAS), GRIMM photoelectric counters, angle-scattering nephelometers, aethalometer, SP-9/6 sun photometer, СЕ 318 Sun-Sky radiometer (AERONET), MS-53 pyrheliometer, MS-802 pyranometer, ASP aureole photometer, SSP scanning photometer, TU-134 Optik flying laboratory, Siberian lidar station, stationary multiwave lidar complex LOZA-M, spectrophotometric complex for measuring total ozone and NO2, multivariable instrument for measuring atmospheric parameters, METEO-2 USM, 2.4 AEHP-2.4m station for satellite data receive. Results of numerical calculations of solar down-fluxes on the Earth’s surface were compared with the values measured in clear air in the summer periods in 2010—2012 in a background region of Siberian boreal zone. It was shown that the relative differences between model and experimental values of direct and total radiation do not exceed 1% and 3%, respectively, with accounting for instrumental errors and measurement error of atmospheric parameters. Thus, independent data on optical, meteorological, and microphysical atmospheric parameters allow mutual intercalibration and supplement and, hence, provide for qualitatively new data, which can explain physical nature of processes that form the vertical structure of the aerosol filed.