Graphene oxide (GO), consisting of numerous oxygen functional groups and 2-D graphene sheet, has drawn intensive attention as a promising membrane material due to its molecular-sieving nanochannel and ease of scale up. However, GO membranes have generally showed a low gas permeability stemming from the high tortuosity of laminate structure. Herein, we prepared silica/GO hybrid membranes to overcome the low gas permeability of GO membrane by tuning its surface area and interlayer spacing. The size of silica nanoparticles grown on the GO nanosheets was successfully controlled by varying the concentration of silica precursor. In particular, the relationship between gas permeability of silica/GO hybrid membranes and the size of silica nanoparticles was investigated.