Atmospheric precipitation acts as a significant pathway for pollutants from the atmosphere to the Earth’s surface, and analyzing urban precipitation data on intensity, fallout regime, transfer patterns, and solid particle content helps identify pollution sources. For the first time in the Moscow megacity, the levels of soluble forms of potentially hazardous elements (PHEs) in atmospheric precipitation were studied during the whole summer season of May–September 2019. The concentrations of Al, As, B, Ba, Be, Bi, Cd, Ce, Co, Cu, Fe, La, Li, Mn, Ni, P, Pb, Rb, Sb, Sn, Sr, and Zn were determined using inductively coupled plasma mass spectrometry and atomic emission spectroscopy methods. The research underscores the crucial role of atmospheric precipitation in washing PHEs out of the atmosphere. In May and September, concentrations of PHEs surpass the warm-season average. Notable contamination in May stems from elevated traffic during vacations, extensive burning of plant debris and wood, and pollen transport. Summer months are characterized by reduced forest and agricultural fires, traffic, and increased vegetation, leading to lower PHE concentrations, especially in July, with typical amount of precipitation contributing to pollutant dispersion. Elevated PHE levels in September are observed due to increased traffic load, biomass burning, and the expansion of unvegetated soil areas. Rainwater is enriched with Sb, Pb, Cd, Zn, Cu, B, Bi, P, and Sr, sourced from vehicle emissions, soil particles, industry, construction dust, biomass burning, and forest fires. Moderate enrichment with Ba, Mn, Ni, Co, and Sn also occurs episodically. Regression analysis highlights solid particles’ role as a major PHE source in rainwater, with the longer antecedent dry periods and the higher acidity level of rain intensifying the accumulation of PHEs. Long-range transport plays a lesser role, with Southern and Northern Europe, Western Siberia, and the central part of European Russia contributing meaningfully.