Samples of atmospheric depositions from five types of functional areas in Shijiazhuang, Hebei Province, China, were collected, and the concentrations of six toxic heavy metals (Cd, Cr, Cu, Pb, Ni, and Zn) were measured. Geographic information system, Pb isotope assessment, multivariate statistical analysis (principal component analysis, PCA), the geoaccumulation index (Igeo), potential ecological risk index (PERI), and a health risk assessment model were used to study the degree of pollution, identify sources of pollution, and assess the health risks to children and adults via three pathways (hand–mouth intake, skin contact, and respiration). The results show that the high traffic volume and exhaust gas emissions have led to high concentrations of heavy metals. The Igeo and PERI values of Cd (0.38–2.0 and 108–4531, respectively), indicating the present high pollution level and potential risk, respectively, varied the most. Pb isotope and PCA showed that Pb, Zn, and Cd from atmospheric deposition come from power plants and traffic—Cu is related to traffic, and Ni and Cr come mainly from soil particles (natural source). The health risk assessment showed that heavy metals in atmospheric depositions are at a safe level in the study area.