Wind　turbine　blades　made　of　glass　fiber-reinforced　polymer　(GFRP)　are　subjected　to　harsh　conditions,　including　high-speed　raindrop　impact.　The　poor　peel　and　impact　resistance　of　the　untoughened　GFRP　composites　severely　shortens　the　service　life　of　the　turbine　blades.　Enhancing　GFRP　toughness　requires　innovative　approaches.　Core-shell　particles　(CSPs)　can　significantly　enhance　the　toughness　of　epoxy　resin.　However,　the　toughening　mechanism　of　CSP　in　GFRP　composites　remains　unclear.　This　study　investigates　the　toughening　mechanisms　of　CSPs　in　GFRP,　focusing　on　surface　chemical　modifications　to　optimize　interfacial　interactions.　Glycidyl　methacrylate　(GMA)-modified　(GCSP)　and　silane-modified　CSP　(KCSP)　were　synthesized　to　strengthen　chemical　bonding　with　the　epoxy　matrix　and　mechanical　interlocking　at　fiber　interfaces.　Results　indicate　that　KCSP　demonstrated　superior　performance:　lap　shear　strength,　Mode　I,　and　Mode　II　critical　energy　release　rates　increased　by　68%,　65.1%,　and　32.2%,　respectively,　compared　to　unmodified　GFRP.　At　5　wt%　KCSP　loading,　mass　loss　under　high-pressure　water　impact　decreased　by　90%.　To　investigate　the　toughening　mechanism　of　KCSP,　molecular　dynamics　(MD)　simulations　were　conducted　to　elucidate　the　mechanisms　underlying　the　mechanical　and　structural　properties.　©　2025　Wiley　Periodicals　LLC.