The crystal structure of the new inorganic-organic hybrid compound [4-CH 3 C 6 H 4 CH 2 NH 3 ] 2 [CdCl 4 ] has been determined by single crystal X-ray diffraction. The compound crystallizes in the orthorhombic space group Pnma with lattice parameters a = 10.721(2), b = 33.986(6), c = 5.326(1)Å, β = 97.222(1)• , V = 1940.8(7)Å 3 , and Z = 4. The framework of the title compound is built upon layers parallel to (010) made up from corner-sharing CdCl 6 octahedra. 4-Methylbenzylammonium cations are situated between the layers and connect them via an N-H· · · Cl hydrogen bonding network. The Cd atom is located on an inversion centre, and the coordination environment is described as distorted octahedral. Solid state 13 C CP-MAS NMR spectroscopy is in agreement with the X-ray structure. DFT calculations allow the attribution of the carbon peaks to the independent crystallographic sites. Thermal analysis and infrared spectroscopy were also used to characterize the complex.