A series of highly porous 4,8-connected isoreticular MOFs of the scu topology [Cu-4(L-1)(H2O)(4)]center dot 20DEF, [Cu-4(L-2)(H2O)(4)]center dot 16DMF center dot 5H(2)O, and [Cu-4(L-3)(H2O)(4)]center dot 14DMF (L-1-L-3 are (R)-1,1'-binaphthyl-derived octacarboxylate bridging ligands) were synthesized and characterized by single-crystal X-ray crystallography. Although the frameworks exhibit some distortion during the solvent removal process, the high-connectivity nature of the building blocks helps in stabilizing the frameworks, leading to high surface areas (S-BET = 1189-2448 m(2)/g) and significant hydrogen uptake of up to 1.8 wt % (77 K, 1 atm).