The occurrence, distribution, and sources of organochlorine pesticides (OCPs) were investigated using paired soil and pine needle samples from Ulsan, South Korea. Mean total OCP concentrations were 31.3 ± 27.4 ng/g dw in soil (excluding outliers) and 25.9 ± 13.9 ng/g ww in pine needles. In soil, endosulfan (34%) and DDTs (28%) were predominant, whereas hexachlorobenzene (HCB) and endosulfan predominated in pine needles. Metabolites were more abundant in soil, while volatile parent compounds were more prevalent in pine needles. Soil total organic carbon showed significant correlations with PeCB and chlordane-related compounds, whereas lipid content in pine needles exhibited no significant relationship with OCP levels. A novel KOA-based pine/soil air-equivalent ratio indicated that relatively volatile OCPs (e.g., HCB, PeCB, α-, γ-HCH) are primarily influenced by atmospheric processes, whereas legacy compounds are preferentially retained in soil. Elevated air-equivalent signals at industrial sites highlight a stronger atmospheric influence. Diagnostic ratios suggest that OCP contamination mainly reflects historical pesticide use, while mirex, HCB, and PeCB indicate additional contributions from long-range transport and industrial emissions. A soil-based cancer risk assessment identified potential risks primarily driven by p,p′-DDE and HCB. Overall, integrating soil and pine needle data with KOA-based analysis enhances source apportionment and supports more effective monitoring of OCP contamination.