House settled dust (HSD) contains various hazardous materials, including polycyclic aromatic hydrocarbons (PAHs) and metals. Exposure to toxicants contained in HSD is of paramount concern especially in the case of young children, due to their particular behavioral characteristics. In this context, extracts of sieved vacuum cleaner dust from 20 residences with young children were examined for the presence of PAHs and trace metals, in Athens, Greece. The results indicated that PAHs and metals were ubiquitous in the studied residences. The calculated enrichment factors (EF) of trace metals indicated that Cu, Se, Zn, Hg, Cd, and Pb were mainly of anthropogenic. According to the PCA analysis, the main sources of household dust were: smoking inside the houses, combustion processes, resuspension of soil dust, and vehicle traffic. In general, the cancer risk due to PAHs exposure was found lower than the threshold value. The ingestion of house dust was the most important route of exposure to metals. The dose of almost all elements for the children was found 1–2 orders of magnitude lower than the corresponding reference values. Both the carcinogenic and noncarcinogenic risks of exposure were within the safety limits.