The cyano-bridged 3D heteronuclear polymeric complex, [Cd(NH3)(mu-ampy)Ni(mu-CN)(4)](n), (1) (ampy = 3-aminomethylpyridine), has been synthesized and characterized by FT-IR and Raman spectral, thermal and elemental analyses. The crystal structure of 1 has been determined by X-ray single crystal diffraction. The complex crystallizes in orthorhombic system with space group Pnma. In 1, Ni(II) ion is five coordinated with square-pyramidal geometry defined by the four C atoms from the four symmetry related cyano ligands and one N atom from the ampy ligand. The Cd(II) ion adopts slightly distorted octahedral coordination geometry completed by the six N atoms from one ammine, one ampy and four cyano ligands. The [Ni(CN)(4)](2-) anion is coordinated to the adjacent four Cd(II) ions to generate a Cd-Ni(CN)(4) 2D undulate layer. The adjacent 2D layers are connected by the mu-ampy bridging ligands to form a 3D pillar-layered framework.