In order to improve the safety of 2,4,6,8,10,12-hexanitro-2,4,6,8,10,12hexaazaisowurtzitane (CL-20) while preserving its high energy yield, a nanocomposite containing CL-20 and 1,3,5-triamino-2,4,6-trinitrobenzene (TATB) with a particular structure is prepared using an facile and fast antisolvent crystallization method. Using this approach, which takes advantage of strong antisolvent and temperature effects, a lamellar arrangement structure is created consisting of nanosheets containing CL-20 and TATB, and further coated with dendritic nanometer-scale TATB. XRD and Raman spectra indicate that CL-20 in the resulting nanocomposite takes the form of α polymorph owing to the presence of ultrapure water. The HPLC results show that the TATB content of the nanocomposite is 20.2 wt%. When the surface coating of TATB is removed, 8 wt% TATB remains between the internal nanosheets. Due to the multiple desensitization effects of this structure, the nanocomposite has much lower sensitivity, roughly comparable to that of the insensitive explosive LLM-105. Thermal analysis by thermogravimetry (TG) and differential scanning calorimeter indicates that the thermal decomposition activity of the nanocomposite is higher than those of raw materials, and in addition, its thermal stability is greater.