This paper reviews the results of several prior studies to highlight how the concept of the metal-organic framework/graphite oxide (MOF/GO) composites was developed towards their application as separation media for small molecule gases at ambient conditions. The studies are analyzed from a surface engineering standpoint. The MOF/GO composites have been developed considering both the advantages and drawbacks of the composite components: MOF provided a high porosity and reactive centers and GO a dense array of carbon atoms to increase dispersive interactions. The resulting materials showed a significant enhancement in porosity owing to the formation of pores at the interface of GO and MOF crystals. GO oxygen groups were identified as nucleation sites for the formation of the MOF crystals. Other heteroatoms like N also contributed to that effect and could positively enhance the composites structural/chemical heterogeneity. That heterogeneity governed the excellent performance of the composites as reactive adsorbents of NH3, H2S, NO2 and physical adsorbents of CO2 at ambient conditions. While the MOF structure collapsed upon exposure to toxic gases, it was preserved after CO2 adsorption indicating the recyclability of these materials. Systematic studies of the composite properties showed that such factors as the GO level of oxidation, flake sizes of a graphite precursor and the geometry of MOF crystals are of paramount importance dictating the final morphology of the composite. The properties of the composites make them potentially suitable for gas sensing or energy harvesting. (C) 2014 Elsevier Inc. All rights reserved.