Abstract The electron-proton co-operation in organic-inorganic hybrid systems, [Pd(H2-x EDAG) (HEDAG)] · TCNQ and [Pt(H2-x DAG) (HDAG)] · TCNQ complexes, leads to two different types of the metal-insulator transition, which originate in the instability of the 1-D π electronic state of the TCNQ stacks. Here, HDAG or HEDAG stands for hydro-or hydroethylene-diaminoglyoxime. Their driving forces are attributable to freezing of the fluctuation of protons in the interchain H-bonds and the charge transfer from the [Pt(H2-x DAG) (HDAG)] metal complex to TCNQ stacks, respectively.