Crystals of cadmium zinc diborate, Cd1.17Zn0.83B2O5, have been obtained by spontaneous nucleation in a platinum crucible at 1072 K. The crystal structure exhibits diborate groups, B2O54−, sharing O atoms with considerably distorted M1O6 octahedra and M2O4 tetrahedra. Both metal centers are disordered in the proportion Cd:Zn = 0.92:0.08 on the M1 site and Cd:Zn = 0.25:0.75 on the M2 site. A strong second-harmonic generation has been observed for the title compound when excited with an Nd:YAG laser (λ = 1064 nm).