Here we report on the synthesis of a graphene/polyaniline (PANI) nanocomposite and its application in the development of a hydrogen (H2) gas sensor. Using a chemical synthetic route, graphene was prepared and ultrasonicated with a mixture of aniline monomer and ammonium persulfate to form PANI on its surface. The developed material was characterized by scanning electron microscopy (SEM), transmission electron microscopy, Raman spectroscopy, and X-ray photoemission spectroscopy. The SEM study revealed that the PANI in the composite has a nanofibrillar morphology. We investigated the H2 gas sensing performance of this material and compare it with that of the sensors based on only graphene sheets and PANI nanofibers. We found that the graphene/PANI nanocomposite-based device sensitivity is 16.57% toward 1% of H2 gas, which is much larger than the sensitivities of sensors based on only graphene sheets and PANI nanofibers.