By the present a large amount of data has been accumulated on direct measurements of the pollution and thermodynamic state of the atmosphere in the Moscow region, which was obtained at stations of Roshydromet, Mosecomonitoring, A.M.Obukhov Institute of Atmospheric Physics (OIAP), M.V. Lomonosov Moscow State University, NPO Typhoon, what allows estimating pollution emissions based on measurements and correcting existing emission inventories, which are evaluated mainly on indirect data connected with population density, fuel consumption, etc. Within the framework of the project, the whole volume of data on the concentration of ground contaminants CO, NOx, SO2, CH4, obtained at regularly operated Moscow Ecological Monitoring stations and at OIAP stations from 2005 to 2014, was systematized. Observation data on pollution concentrations are supplemented by measurements of their integral content in the atmospheric boundary layer, obtained by differential spectroscopy methods (MAX DOAS, ZDOAS) at stationary stations and by passing Moscow with DOAS-equipped car. The paper present preliminary estimates of pollution emissions in the Moscow region, obtained on the basis of the collected array of experimental data. The estimations of pollutant emissions from Moscow were obtained experimentally in a few ways: (1) on the basis of network observations of surface concentrations, (2) on the basis of measurements in the atmospheric layer 0–348 m at Ostankino TV tower, (3) on the basis of the integral pollutant (NO2) content in ABL obtained by DOAS technique from stationary stations, and (4) using a car with DOAS equipment traveling over the closed route around Moscow (for NO2). All experimental approaches yielded close values of pollution emissions for Moscow. Trends in emissions of CO, NOx, and CH4 are negative, and the trend of SO2 emission is positive from 2005 to 2014.