The design, synthesis, and structural characterization of two microporous metal-organic framework structures, [M(bdc)(ted)(0.5)]center dot 2 DMF center dot 0.2 H2O (M = Zn (1), Cu (2); H(2)bdc 1,4-benzenedicarboxylic acid; ted = triethylenediamine; DMF: N,N-dimethylformamide) is reported. The pore characteristics and gas sorption properties of these compounds are investigated at cryogenic temperatures, room temperature, and higher temperatures by experimentally measuring argon, hydrogen, and selected hydrocarbon adsorption/desorption isotherms. These studies show that both compounds are highly porous with a pore volume of 0.65 (1) and 0.52 cm(3) g(-1) (2). The amount of the hydrogen uptake, 2.1 wt % (1) and 1.8 wt % (2) at 77 K (1 atm; 1 atm = 101 325 Pa), places them among the group of metal-organic frameworks (MOFs) having the highest H-2 sorption capacity. [Zn(bdc)(ted)(0.5)]center dot 2 DMF center dot 0.2 H2O adsorbs a very large amount of hydrocarbons, including methanol, ethanol, dimethylether (DME), n-hexane, cyclohexane, and benzene, giving the highest sorption values among all metal-organic based porous materials reported to date. In addition, these materials hold great promise for gas separation.