We summarized detailedly in this review the basic theory of quantum chemistry, and discussed the methods for calculating key parameters of energetic materials (density, heat of formation, detonation heat, detonation velocity, detonation pressure and impact sensitivity). We also compared the characteristics and applicable scope of these methods. In addition, the application of CHEETA, EXPLO5 and other computing software in the field of energetic materials were briefed. Finally, in order to satisfy the comprehensive requirements for new generation materials, high energy, good stability and environmental friendliness, we designed 20 new high nitrogen molecules, and estimated their physicochemical properties and energetic parameters using the quantum chemistry methods as mentioned above. The design concept and principle for the new energetic compounds was put forward. It was expected that it would promote the development of energetic materials. Seventy-six references were contained.