This study investigated the accumulation of total phosphorus (TP) and heavy metals (HMs; Pb, Zn, Cu, Cd, Cr, and Ni) in citrus orchard soils in Jeju Island, Korea, identifying potential soil pollution sources using statistical analysis. Anthropogenic HM pollution was evaluated using the geoaccumulation index and enrichment factors, whereas HM bioavailability was assessed via single extraction. TP, Zn, Cu, and Cr concentrations in citrus orchard topsoil were significantly higher than those in forestland soils, indicating their accumulation in the surface layer. Statistical analyses confirmed that elements with high concentrations were closely related to potential pollution sources accumulated on the surface layer of citrus orchards owing to agricultural activities. Particularly, Zn and Cu accumulation was confirmed to originate from intensive compost and pesticide use in citrus orchards. Cu showed the highest contamination and enrichment of all HMs. However, Zn and Cu fractions, determined via an availability assessment, were dominated by acid or complex compounds, indicating that labile Zn and Cu have potential bioavailability for plants. Nevertheless, their fractions accounted for a small proportion (mean < 15%). Therefore, despite the high pollution levels of Zn and Cu, their availabilities were extremely low, indicating a negligible bioavailability in crops and no impact on aquatic ecosystems.