A simple, promising, environmentally friendly, and high yield technique to synthesize high specific surface area (SSA) and porous graphene-like materials from glucose precursor through carbonization and controlled chemical iron chloride (FeCl3) activation was demonstrated. Designing this nanoporous graphene-based adsorbent with high SSA, abundant micropore volume, tunable pore size distribution, and high adsorption capacity, is crucial in order to deal with the demands of large-scale reversible natural gas storage applications. Raman spectroscopy, BET method of analysis, and N2 adsorption/desorption measurements at -196 °C were adopted to evaluate the structural and textural properties of the resultant glucose derived-graphene (gluGr) samples. The effects of different carbonization conditions, such as the inert environments (argon, helium, and argon) and temperatures (700, 800, 900, and 1,000 °C), have been studied. A glucose-derived graphene carbonized under nitrogen environment at 700 °C (NGr700) with highly interconnected network of micropores and mesopores and large SSA (767m2/g) exhibited excellent methane (CH4) storage property with exceptionally high adsorption capacity, superior to other glucose-derived graphene (gluGr) samples. A maximum volumetric capacity up to 42.08 cm3/g was obtained from CH4 adsorption isotherm at 25 °C and 35 bar. Note that the adsorption performance of the CH4 is highly associated with the SSA and microporosity of the gluGr samples, especially NGr700 that was successfully synthesized by FeCl3 activation under N2 environment.