The poor bonding of energetic crystals has severely influenced the comprehensive performance of explosive composites. Herein, surface modification is displayed as an effective method to implement the interaction of composites. In this work, a multipurpose functionalization of interfacial additives and biomimetic coating was demonstrated in facial and reproductive ways. The self-polymerization of dopamine (DA) formed polydopamine (PDA) shells, followed by neutral bonding agent (NBA) grafting, which led to a roughness change of the 1,3,5-triamino-2,4,6-trinitrobenzene (TATB) crystal. The new bonds of amino ester (-NHCOO) were generated, proving the success of the "grafting to" strategy. The ability to resist deformation after surface modification was significantly improved with strain below 0.06% under 75 °C or 9 MPa. The storage modulus of PBX is above 4000 MPa within a temperature range of 20-120 °C. Moreover, the mechanical properties of PBX-3 significantly improved, with the strength and elongation in the Brazillian mechanical test increasing by 19.4 and 24.4%, respectively, ultimately resulting in an enhancement of approximately 51.6% in fracture work. The dual effect of hydrogen bonding and a physical anchor may serve to enhance mechanical properties. The approach of PDA coating and NBA grafting presented in this paper may be favorable for improving the mechanics of general composites.