Polymer–crystal composite particles formed by crystals coated with binders are widely used in the fields of medicine, energy, the chemical industry, and civil engineering. Binder content is an important factor in determining the mechanical behavior of composite particles. Therefore, this study aimed to investigate the underlying effect of binder coatings in the fracture micromechanics of polymer–crystal composite particles using the discrete element method (DEM). To achieve this objective, realistic particle and crystal shapes were first obtained and reconstructed based on X-ray micro-computed tomography (μCT) scanning and scanning electron microscope (SEM) images. A series of single particle crushing tests and DEM simulations were conducted on real and reconstructed polymer–crystal composite particles, respectively. Based on the experimental and DEM results, the effect of binder coatings on the crushing strength and crushing patterns of polymer–crystal composite particles was measured. Moreover, the micromechanics of the development and distribution of microcracks was further investigated to reveal the mechanism by which binder coatings affect polymer–crystal composite particles.