The dataset provides raw data on key properties in the text as well as raw data on the temperature and energy balances of the P, P1, P2, P3 and P4 systems at room temperature. These data allow the results obtained in the article to be reproduced, while the reader can obtain the raw data for the plots not labeled with data in the article and thus quantify the exact magnitude of the changes shown in the plots. The main work of the article is: Molecular dynamics (MD) simulations have been applied to investigate 1, 1-diamino-2, 2-dinitroethene (FOX-7) crystal and FOX-7(011)-based polymer-bonded explosives (PBXs) with four typical polymers, polyethylene glycol (PEG), fluorine-polymer (F₂₆₀₃), ethylene-vinyl acetate copolymer (EVA) and ester urethane (ESTANE5703) under COMPASS force field. Binding energy (E_bind), cohesive energy density (CED), initiation bond length distribution, radial distribution function, and isotropic mechanical properties of FOX-7 and its PBXs at different temperatures were reported for the first time, and the relationship between them and sensitivity. Using quantum chemistry, FOX-7 was optimized with the four polymers at the B3LYP/6-311++G(d,p) level, and the structure and RDG of the optimized composite system were analyzed.