Per- and polyfluoroalkyl substances (PFAS) are persistent environmental contaminants highly resistant to chemical, physical, and biological degradation. The application of sustainable organic amendments such as biochar has emerged as a promising strategy to reduce PFAS bioavailability and accumulation in crops. The aim of this study was to evaluate the potential of biochar-amended vermicompost (vermichar) to improve the quality of soils exposed to substantial PFAS inputs. To this end, an arid soil collected from abandoned agricultural land in the Canary Islands (Spain) was amended with vermichar at 5%, 10%, and 20% (w/w, dry weight basis) and subsequently spiked with a PFAS mixture (25 ng g⁻¹ dry soil each) comprising short-chain (PFPeA), long-chain (PFOS and PFOA), and emerging (6:2 FTSA) compounds. Lettuce (Lactuca sativa) and chickpea (Cicer arietinum) were grown in treated soils for two months. Following harvest, plant growth parameters, soil microbial activity, exo-enzyme activities, nutrient availability (NH₄⁺, NO₃⁻, and inorganic P), and PFAS concentrations were determined. Vermichar application progressively increased soil enzyme activities, likely due to its high enzymatic and organic matter content. Notably, PFAS-contaminated soils amended with vermichar exhibited significantly greater N- and P-acquiring enzyme activities than non-contaminated soils, consistent with effective PFAS immobilization and limited interference with soil microbial processes. NH₄⁺ concentrations declined across all treatments, whereas NO₃⁻ availability increased substantially following vermichar application, particularly in PFAS-free soils. PFAS analyses further revealed a significant reduction in plant uptake in vermichar-amended treatments. However, the highest application rate (20% w/w) adversely affected chickpea growth, indicating potential phytotoxic effects at excessive doses. Overall, vermichar application at rates of 10% (w/w) or lower simultaneously enhanced soil fertility and reduced PFAS bioavailability and plant uptake, highlighting its potential as a sustainable remediation strategy for PFAS-contaminated agricultural soils.