The present study successfully synthesized a novel biochar adsorbent (M−L−BC) using litchi seed modified with zinc chloride for PFASs removal in water. M−L−BC greatly enhanced removal of all examined PFASs (>95 %) as compared to the pristine biochar (<40 %). The maximum adsorption capacity was observed for PFOS, reaching 29.6 mg/g. Adsorption kinetics of PFASs followed the pseudo-second-order model (PSO), suggesting the predominance of chemical adsorption. Moreover, characterization and density functional theory (DFT) calculations jointly revealed involvement of surface complexation, electrostatic interactions, hydrogen bonding, and hydrophobic interactions in PFAS adsorption. Robust PFAS removal was demonstrated for M−L−BC across a wide range of pH (3–9), and coexisting ions had limited impact on adsorption of PFASs except PFBA. Furthermore, M−L−BC showed excellent performance in real water samples and retained reusability after five cycles of regeneration. Overall, M−L−BC represents a promising and high-quality adsorbent for efficient and sustainable removal of PFASs from water.