Two new metal-organic frameworks (MOF), [(CuCN)2·(6-mquin)2] (1) and [Me3SnCu(CN)2·(quina)2(H2O)2] (2) (6-mquin = 6-methyl quinolone, quina = quinaldic acid) were synthesized and characterized. Single crystals of MOF 1 were characterized by IR and NMR spectroscopy, as well as X-ray single crystal analysis. The structure of MOF 2 was studied by IR and NMR spectroscopy as well as computational studies. The structure of MOF 1 consists of 1D (CuCN)n chains, whereas the 6-mquin ligands alternate on both sides of the chain. Hydrogen bonds play an essential role for the construction of the 3D network structure. On the other hand, the theoretical structural analysis of MOF 2 indicated that the Cu(CN)2 fragments represent the main building blocks of the structure, which are bridged by the Me3Sn+ cations to construct 1D infinite parallel zigzag chains. MOFs 1 and 2 were used as heterogeneous catalysts for the oxidative discoloration of methylene blue dye (MB) by H2O2.