We studied the 60Co gamma-ray radiolysis of thiocyanate aqueous solutions in the presence of free radical scavengers, determination of cyanide of radiated thiocyanate solutions, degradation of cyanide and thiocyanate complicated system and cyanide, thiocyanate and copper (I) cyanide complicated system. The presence of NaHCO3 and n-butanol made the degradation efficiency of thiocyanate decreased, in the radiation procession of thiocyanate, cyanide was produced; and the possible reaction equation is SCN(-) + 8*OH-->SO4(2-) + CN(-) +4H2O, in the cyanide and thiocyanate system, the thiocyanate degradation rate can obtained 30%, free cyanide degradation was little effected by coexistence of thiocyanate; and due to strong complex ability of copper (I), the main form of copper (I) cyanide is Cu(CN)3(2-), the total cyanide of the system can't be degraded completely and degradation rate is about 80%.