This study proposes a method utilizing nano-SiO2 modified polyvinyl alcohol fibers to enhance the interface properties of geopolymer concrete. The surface properties of modified polyvinyl alcohol fibers were analyzed through microscopic characterization. The influence of different dosages of modified polyvinyl alcohol fibers on the mechanical properties of geopolymer concrete was investigated. Molecular dynamics simulations revealed the interfacial toughening mechanism between modified polyvinyl alcohol fibers and geopolymer concrete. Results showed that nano-SiO2 modified polyvinyl alcohol fibers increased surface roughness, thereby enhancing interfacial adhesion and mechanical interlocking between fibers and geopolymer concrete, significantly improving compressive, splitting tensile, and flexural strengths of geopolymer concrete with an optimal fiber dosage of 0.2 %. Relative to unmodified PVA fibers, the modified fibers enhance the compressive, splitting tensile, flexural strength, and elastic modulus by 20.19 %, 15.72 %, 22.34 %, and 30.58 % respectively. KH560 serves as an intermediate medium for nano-SiO2 modified polyvinyl alcohol fibers, generating numerous hydrogen bonds at the interface and tightly adhering nano-SiO2 to the surface of polyvinyl alcohol fibers. Additionally, nano-SiO2 can form ionic bonds and stable Si-O-Si bonds with the hydrated sodium aluminosilicate gel.