AbstractThis study reveals double plasma modification of ultra‐high molecular weight polyethylene (UHMWPE) fibers by oxygen/argon duoplasmatron source to investigate the synergistic effect of double plasma mixture on the mechanical performance of UHMWPE/vinyl ester laminated composites. The single‐factor experiment was used to determine the preparation process parameter range. The modified fiber was characterized and mechanical properties of UHMWPE/vinyl ester composites were evaluated. The results showed that the UHMWPE fiber modified by double plasma treatment with oxygen/argon duoplasmatron source exhibited more hydroxyl groups than untreated fiber and the single plasma‐modified fiber with oxygen source, and the surface water adsorb capacity was significantly improved, which contributed to the combination of resin and fiber surface. The tensile strength of the composite with double plasma modification increased to 380.48 MPa, which was higher than untreated and oxygen plasma treated samples by 36.9% and 18.9%, respectively. The GIC value was even 78.1% higher than that of oxygen plasma‐treated sample, and the interlaminar shear strength was increased by 19%. In terms of low‐velocity impact response, the absorbed energy of double plasma modified composites was increased, confirming that the mechanical resistant performance was enhanced by the modification with oxygen/argon duoplasmatron source.