The present study aims to demonstrate the effects of horizontal grid resolution on the simulated pollution concentration fields over Bulgaria. The computer simulations are performed with a set of models used worldwide—the Weather Research and Forecasting Model (WRF)—the meteorological preprocessor, the Community Multiscale Air Quality Modeling System (CMAQ)—chemical transport model, Sparse Matrix Operator Kernel Emissions (SMOKE)—emission model. The large-scale (background) meteorological data used in the study were taken from the ‘NCEP Global Analysis Data’ with a horizontal resolution of 1° × 1°. Using the ‘nesting’ capabilities of the WRF and CMAQ models, a resolution of 9 km was achieved for the territory of Bulgaria by sequentially solving the task in several consecutive nested areas. Three cases are considered in this paper: Case 1: The computer simulations result from the domain with a horizontal resolution (both of the emission source description and the grid) of 27 km.; Case 2: The computer simulations result from the domain with a horizontal resolution (both of the emission source description and the grid) of 9 km.; Case 3: A hybrid case with the computer simulations performed with a grid resolution of 9 km, but with emissions such as in the 27 km × 27 km domain. The simulations were performed, for all the three cases, for the period 2007–2014 year, thus creating an ensemble large and comprehensive enough to reflect the most typical atmospheric conditions with their typical recurrence. The numerical experiments showed the significant impact of the grid resolution not only in the pollution concentration pattern but also in the demonstrated generalized characteristics. Averaged over a large territory (Bulgaria); however, the performances for cases one and two are quite similar. Bulgaria is a country with a complex topography and with several considerably large point sources. Thus, some of the conclusions made, though based on Bulgarian-specific experiments, may be of general interest.