There has been a steady growth in research on porous materials such as metal−organic frameworks (MOFs) for their various applications. A significant drawback of conventional MOF synthesis is the use of toxic organic solvents to solubilize various organic linkers. Such an approach requires a longer MOF growth time and energyintensive solvent recovery schemes during scale-up. In this work, we report the synthesis of Fe, Cu-based MOFs using trimesic acid (1,3,5benzene tricarboxylic acid) as a linker via a facile aqueous medium route under environment-friendly conditions without requiring any toxic organic solvent and temperature. NaOH was used as a stoichiometric deprotonating agent for the aromatic carboxylic acid groups in the linker to facilitate linker solubility and interaction with metal ions. The aqueous medium-synthesized MOFs showed improved gas sorption characteristics compared with the same materials synthesized under the conventional solvent-mediated route. The synthesized MOFs were characterized by Brunauer−Emmett−Teller, powder X-ray diffraction, scanning electron microscopy, thermogravimetric analysis, Fourier transform infrared, and X-ray photoelectron spectroscopy, and isotherms were measured for different gases (CO 2 , CH 4 , N 2 , propylene, and propane). Ideal adsorbed solution theory was used for binary selectivity calculations for gas systems such as CO 2 / CH 4 , CH 4 /N 2 , CO 2 /N 2 , C 3 H 6 /N 2 , and C 3 H 6 /C 3 H 8 . Density functional theory calculation was made to get an insight into the adsorptive behavior of the different gas molecules on the MOFs as adsorbent.