The crystal growth, space group and Raman spectra of the zinc cadmium tetrathiocyanate (ZCTC) single crystal are introduced. The experiments show that the characteristic lattice vibrational modes of ZCTC crystal arises mainly from the internal vibrations of the SCN, ZnN 4 , and CdS 4 groups. These modes are assigned as v 1 (160 cm - 1 , a doubly degenerate CdS 4 bending vibration), v 2 (230 cm - 1 , a doubly degenerate ZnN 4 bending vibration), v 3 (449 cm - 1 , an NCS symmetrical bending vibration), v 4 (474 cm - 1 , an NCS asymmetrical bending vibration), v 5 (794 cm - 1 , a CS stretching vibration), and v 6 (2179 cm - 1 , a CN stretching vibration), respectively. The three-dimensional network structure of ZCTC crystal is identified, and the high nonlinearity of the crystal is mainly attributed to the conjugated charge-transfer bridges( Cd S C N Zn ) that connect all the distorted tetrahedron ZnN 4 and CdS 4 together.