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The emergence of TKX-50, an energetic ionic salt with a high enthalpy of formation and low sensitivity, has opened a new path for the development of high-energetic, insensitive composite explosives. However, due to the poor interfacial binding properties of TKX-50 with conventional binders, there is a lack of effective guidance for the design of TKX-50 based composite explosives. To address the above issues, the interactions between carboxymethyl cellulose acetate butyrate (CMCAB) and other binders with explosives TKX-50/HMX were compared using the molecular dynamics method. Based on the simulations, TKX-50/HMX/CMCAB-based polymer-bonded explosives (PBXs) were prepared with CMCAB as binder, which displays a high binding energy (Ebind) with TKX-50 and high cohesive energy density (CED), and the effect of TKX-50 content on the performance of PBXs was investigated. The physical properties of PBXs, specifically the morphology, mechanical sensitivity, and thermal conductivity, were analyzed by SEM, sensitivity apparatus, and thermal conductivity meter, respectively. The specific heat capacity (Cp) and non-isothermal decomposition temperature of PBXs were tested by DSC, and then the corresponding thermal kinetic parameters were analyzed to evaluate their thermal safety. The adiabatic thermal decomposition processes of PBXs were tested using an ARC instrument. The decomposition mechanism and kinetics were also explored to further analyze their thermal stability and thermal safety under adiabatic conditions. The computer code EXPLO5 was used to predict the detonation parameters of PBXs. The results showed that CMCAB and TKX-50 displayed favorable interfacial bonding properties, and TKX-50 can be bonded with HMX to form a molding powder with a desirable morphology and safety profile. The TKX-50 in PBXs effectively improves the mechanical sensitivity and thermal safety of PBX and has a significant effect on the detonation performance of PBX. This research demonstrates a novel method suitable for screening and investigating high-energetic insensitive explosive systems compatible with TKX-50.