With the aid of a pyridyl tetracarboxylate ligand, 2,5-bis(2',5'-dicarboxylphenyl)pyridine (H4L), two indium-organic frameworks, [In2(L)(OH)2]·2DMF·2H2O (1) and [Me2NH2][In(L)]·2.5NMF·4H2O (2), with (6,8)- and (4,4)-connected nets have been constructed in different solvent systems. Both 1 and 2 exhibit high thermal and chemical stability. Gas sorption behavior of 1 and 2 for N2, C2H2, C2H4, CO2, and CH4 indicate excellent separation selectivities of C2Hx/CH4 and CO2/CH4. Furthermore, 1 possesses a high density of Brønsted sites and shows efficient catalytic conversion for CO2 cycloaddition with epoxides. Meanwhile, luminescence investigations reveal that 2 can detect nitrofurazone efficiently.