The high elasticity and excellent gas barrier properties of rubber composites make them irreplaceable in the field of sealing. Constructing a complicated barrier network to reduce free volume is crucial to improving gas barrier properties. In this research, liquid acrylonitrile-butadiene rubber/γ-Methacryloxypropyl trimethoxy silane (KH570) modified graphene oxide/butyl rubber composites (LNBR/KGO/IIR) were fabricated. A KGO lamellar network was constructed to resist gas diffusion in the IIR matrix. Meanwhile, LNBR macromolecules further occupied the free volume inside the IIR composites, thereby maximizing the retardation of the path of small molecule gas permeation. The modification of GO by KH570 was successfully demonstrated through FTIR and XRD. The grafting rate of KH570 was calculated to be approximately 71.4%. KGO was well dispersed in IIR due to emulsion compounding and the formation of lamellar networks. The 300% modulus, tensile strength and tear strength of KGO/IIR were improved by 43.5%, 39.1% and 14.8%, respectively, compared to those of the IIR composite. In addition, the introduction of LNBR resulted in a 44.2% improvement in the gas barrier performance of nitrogen permeability relative to the original IIR composite.