AbstractSimulations of two mesoscale convective systems (MCSs) that occurred during the Midlatitude Continental Convective Clouds Experiment were performed to examine the impact of aerosol number concentration on the vertical distributions of liquid and ice condensate and the macrophysical, microphysical, and radiative properties of the cirrus‐anvil cloud shield. Analyses indicate that for an increase in aerosol concentration from a clean continental to a highly polluted state, there was an increase in the rime collection rate of cloud water, which led to less lofted cloud water. Aerosol‐induced trends in the cloud mixing ratio profiles were, however, nonmonotonic in the mixed phase region, such that a moderate increase in aerosol concentration produced the greatest reduction in cloud water. Generally, less lofted cloud water led to less anvil ice mixing ratio but more numerous, small ice crystals within the anvil. In spite of reduced anvil ice mixing ratio, the anvil clouds exhibited greater areal coverage, increased albedo, reduced cloud top cooling, and reduced net radiative flux, which led to an aerosol‐induced warming (reduced cooling) effect in these squall lines.