This paper aims to assess the pollution by determining the sources of persistent organic pollutants (POPs) in 22 rural Roma communities in Transylvania in order to assess the human health risk associated with this exposure. For this, 16 polycyclic aromatic hydrocarbons (PAHs), 20 organochlorine pesticides (OCPs) and 12 polychlorinated biphenyls (PCBs) were determined in 22 soil samples collected from selected areas by gas chromatography coupled with mass spectrometry for PAHs and with electron capture detector for all halogenated compounds. Target compounds were isolated from soil by ultrasound-assisted extraction. We found that POP concentrations in soil ranged from 4.86 to 451.85 ng/g dw for PAHs, from 25.62 to 139.30 ng/g dw for OCPs, and from 0.22 to 49.12 ng/g dw for PCBs. The diagnostic ratios ƩLMW/ƩHMW, ANT/(ANT + PHE), and FLT/(FLT + PYR) strongly suggest a pyrogenic model of PAHs, such as biomass, coal, and petroleum combustion, while the isomer ratios ƩDDT/ƩHCH, α-HCH/γ-HCH and (DDE + DDD)/ƩDDT suggest that OCP residues originate from their ancient uses. Non-carcinogenic (HI) and carcinogenic (CR) risks of these organic compounds present in the soil through non-dietary pathways were in the very low-risk category (ranging from 10−8 to 10−4), indicating an absence of these risks from the investigated POPs in the studied area.