An innovative design of a molecularly imprinted phase-change microcapsule (MIM) system for bifunctional applications in waste heat recovery and targeted pollutant removal was reported in this work. This molecularly imprinted system was successfully constructed by encapsulating n-eicosane with a SiO2 base shell through emulsion-templated interfacial polycondensation and then coating a molecularly imprinted polymeric layer with bisphenol A (BPA) as a template molecule through surface free-radical polymerization. The morphology, microstructure, and chemical structure of the resultant molecularly imprinted phase-change microcapsules (MIMs) were characterized, and their phase-change behavior, thermal energy-storage performance, and selective adsorption capability were investigated intensively. The MIMs developed in this study achieved an outstanding latent heat-storage capability with a high capacity more than 165 J/g and also showed an excellent phase-change reliability with a very small fluctuation in phase-change temperatures and enthalpies after 500 thermal cycles. Moreover, the MIMs also presented a high thermal stability over 200 degrees C and good shape stability up to 120 degrees C. Most of all, an effective specific recognition capability and high recognition efficiency were achieved for the MIMs due to the formation of BPA-molecular imprinting sites on their surface. As a result, the MIMs exhibited good adsorption selectivity toward the BPA molecules and satisfactory reusability for targeted removal of BPA with a removal efficiency of 61.7% after 10 cycles of the rebinding-elution procedure. In view of a smart combination of thermal energy-storage and selective adsorption functions, the MIMs developed in this study demonstrate a great potential in applications for waste heat recovery and targeted pollutant removal of industrial and domestic wastewaters.