An interpenetrated indium pyridylcarboxylate framework, [NH2(CH3)(2)][In-(L)(2)]center dot 2.5DMF center dot 5H(2)O (1), has been synthesized by employing a pyridylcarboxylate ligand, 4-(3-carboxylphenyl)picolinic acid (H2L), and an In3+ ion, with both chemical stability and framework flexibility. The desolvated 1 exhibits an uncommon breathing sorption behavior and shows highly selective adsorption for C2H2, C2H4, and CO2 over CH4. Furthermore, 1 shows rapid and higher adsorption efficiency for methylene blue and neutral red in aqueous solution.