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This study shows that chitosan (CS) could be highly useful as a coupling agent in phosphate glass fibre/polycaprolactone (PGF/PCL) composites, as it improved the interfacial shear strength by up to 78%. PGFs of the composition 45P₂O₅&#8315;5B₂O₃&#8315;5Na₂O&#8315;24CaO&#8315;10MgO&#8315;11Fe₂O₃ were dip-coated with CS (with a degree of deacetylation &gt;80%) dissolved in acetic acid solution (2% <i>v</i>/<i>v</i>). Different CS concentrations (3&#8315;9 g L^&#8722;1) and coating processes were investigated. Tensile and fragmentation tests were conducted to obtain the mechanical properties of the single fibres and interfacial properties of the PGF/PCL composites, respectively. It was observed that post-cleaning, the treated fibres had their tensile strength reduced by around 20%; however, the CS-coated fibres experienced strength increases of up to 1.1&#8315;11.5%. TGA and SEM analyses were used to confirm the presence of CS on the fibre surface. FTIR, Raman, and X-ray photoelectron spectroscopy (XPS) analyses further confirmed the presence of CS and indicated the protonation of CS amine groups. Moreover, the nitrogen spectrum of XPS demonstrated a minimum threshold of CS coating required to provide an improved interface.