D-A　hybrid　heterostructures　are　an　attractive　class　of　hybrid　complexes　composed　of　semiconducting　organic　and　inorganic　components,　which　make　them　potential　candidates　for　applications　in　the　photoelectric　fields,　particularly　as　photochromic　materials.　Herein,　we　report　that　the　combination　of　metal　cations　(M　=　Zn2+　or　Cd2+),　silicomolybdic　anions,　and　N,N-di(4-pyridyl)-1,4,5,8-　naphthalene　diimide　(DPNDI)via　two　diffusion　methods　(A　and　B)　led　to　four　three-component　D-A　hybrid　heterostructures　with　silicomolybdic　anions　as　electron　donors,　and　one-dimensional　(1-D)　naphthalenediimide　coordination　networks　of　different　metal　cations,　[Zn-2(DPNDI)(2)(H2O)(4)]center　dot(SiMo12O40)　(1-A　and　1-B)　and　[Cd-2(DPNDI)(2)(H2O)(4)]center　dot(SiMo12O40)　(2-A　and　2-B),　as　electron　acceptors.　Although　the　different　diffusion　methods,1-B,2-A　and　2-B,　are　isostructures　with　close　cell　parameters.　Due　to　the　different　ionic　radii　and　electronegativity　of　metal　cations　in　isostructural　1-B　and　2-B,　they　exhibit　different　electron-transfer　photochromic　behaviors.　This　study　paves　a　new　path　for　designing　novel　photochromic　materials　through　such　third-component　metal　cations.