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TAGP provide strong interaction which packing RDX recrystallization, in this strategy, the high energy content and insensitive qy-RDX were obtained. • High density qy-RDX hybrid crystals have been designed and prepared under constraint of TAGP. • TAGP inhibited the growth of RDX molecules (111) and (200) planes, resulting in improved energy density. • 2D TAGP can greatly change the crystal structure of RDX thereby significantly reduced its sensitivity. In this paper, the widely used energetic material RDX had been modified with 2D high nitrogen polymer (TAGP). Various hybrid RDX crystals (qy-RDX) with higher detonation velocity and better thermostability had been obtained as a result of strong intermolecular interactions between TAGP and RDX molecules. The performance of the qy-RDX had been characterized to clarify the inherent mechanisms. It shows that the⊿ H f of qy-RDX could be largely changed in the range of 23.4 kJ kg−1 to 1343.6 kJ kg−1, whereas the density varies only from 1.81 g cm−3 to 1.86 g cm−3. The resulted detonation velocities are in the range of 8725.5 m·s−1 to 9251.8 m·s−1, depending on the content and state of the TAGP dopant. The sensitivity of the resulted qy-RDX is much better than pristine RDX due to improved crystal quality as well as higher concentration of hydrogen bonds. The impact energy is improved from 8.5 J (RDX) to 22 J (qy-RDX-1), whereas the friction sensitivity improves form 130 N to over 360 N for the same case. The E a for thermal decomposition of qy-RDX-1has reduced from 147.8 kJ mol-1 (RDX) to (124.5 kJ mol-1), since TAGP dopant could be considered as active catalytic sites after melting of RDX. [ABSTRACT FROM AUTHOR]