The compatibility between the majority of thermoplastic veils (TPVs) and epoxies is typically poor, owing to the inherently low surface energies of thermoplastics. This tends to largely affect the toughening performance of TPVs as interlayer materials of carbon fibre/epoxy composites. The traditional methods for surface activation of thermoplastics, such as corona discharge, plasma treatment and acid etches, are not applicable to TPVs as they could cause significant damage to the thermoplastic fibres with nano-/micro-scale diameters. Herein, a UV- irradiation technique was proposed to active the surfaces of polyphenylene-sulfide (PPS) veils, that effectively improved their adhesion with epoxies. Consequently, the effects of an improved veil/epoxy adhesion on the mode-I and mode-II fracture behaviour and corresponding fracture mechanisms of the interleaved laminates were investigated. It was found that an improved veil/epoxy adhesion significantly enhanced the toughening performance of the PPS veils for the laminates manufactured by resin transfer moulding of non-crimp fabrics, by introducing additional carbon fibre delamination and significant PPS fibre damage during the fracture process. In contrast, the increased level of veil/epoxy adhesion inhibited PPS fibre bridging during the fracture process of the laminates produced from unidirectional prepregs, and caused considerable adverse effects on the fracture performance.