Contamination levels of the organic horizon of Al–Fe-humus podzols (Albic Rustic Podzols) in the zone affected by atmospheric emissions of the Severonikel smelter (Murmansk oblast) within a 20-yearlong period are compared. The spatiotemporal changes in the total content of heavy metals in the soils in response to a decrease in aerotechnogenic loads have a complicated pattern. As the content of heavy metals in the soils varies widely, the correlation between their amount in the organic soil horizon and the distance from the contamination source is absent. In response to the ninefold decrease in the amount of atmospheric emission of Ni compounds, the bulk content of Ni in the organic horizons of podzols reliably decreased by 2.5 times. The threefold decrease in the emission of Cu compounds proved to be insufficient for a significant decrease in the Cu content in the soils. In 2016, the content of heavy metals in some sampling points even increased in comparison with the earlier periods. The Ni-to-Cu ratio in the soil samples changed significantly. In 1989–1994, bulk forms of heavy metals in the soil samples formed the sequence Ni > Cu > Co; in 2016, it changed to Cu > Ni > Co, which corresponds to the proportions of these metals in the aerial emissions. Under conditions of the continuous input of heavy metals from the atmosphere, the contamination of the organic horizons of podzols with heavy metals remains at the high or very high levels.