Impact by hailstone, volcanic rock, bird strike, or also dropping tools can cause damage to aircraft materials. For maximum safety, the goal is to increase Charpy impact strength (auc) of a carbon-fiber-reinforced thermoplastic polyphenylene sulfide polymer (CFRTP-PPS) composite for potential application to commercial aircraft parts. The layup was three cross-weave CF plies alternating between four PPS plies, [PPS-CF-PPS-CF-PPS-CF-PPS], designated [PPS]4[CF]3. To strengthen, a new process for CFRP-PPS was employed applying homogeneous low voltage electron beam irradiation (HLEBI) to both sides of PPS plies prior to lamination assembly with untreated CF, followed by hot press under 4.0 MPa at 573 K for 8 min. Experimental results showed a 5 kGy HLEBI dose was at or near optimum, increasing auc at each accumulative probability, Pf. Optical microscopy of 5 kGy sample showed a reduction in main crack width with significantly reduced CF separation and pull-out; while, scanning electron microscopy (SEM) and electron dispersive X-ray (EDS) mapping showed PPS adhering to CF. Electron spin resonance (ESR) of a 5 kGy sample indicated lengthening of PPS chains as evidenced by a reduction in dangling bond peak. It Is assumed that 5 kGy HLEBI creates strong bonds at the interface while strengthening the PPS bulk. A model is proposed to illustrate the possible strengthening mechanism.