AbstractDue to its higher overall performance than ordinary concrete, polymer concrete (PC) beam has been widely used in the field of structural engineering. However, it is widely recognized that PC cannot simultaneously achieve the highest mechanical strength and optimal damping performance to reduce vibration during its long‐term service lifetime. To address this contradiction, the effect of various diluents contents on the overall performance of PC was investigated first in this investigation. Experimental findings revealed that the bending strength of PC exhibits an initial increase followed by a decrease with an increment of diluents, while its damping ratio displays an inverse trend. To obtain excellent overall performance (higher flexural strength and damping ratio) of PC, gradient PC has been manufactured by horizontal partition casting process (HPCP) and stereoscopic layered casting process (SLCP). Experimental results demonstrated that the gradient PC manufactured by HPCP exhibited better overall performance compared to SLCP. Furthermore, the graphite and carbon fiber were incorporated into the above gradient PC, and experimental results revealed that the incorporated graphite and carbon fiber can further increase the overall performance of the above gradient PC. Similarly, the incorporation of glass fiber cloth and carbon fiber cloth, along with surface treatment, significantly enhanced the overall performance of PC. The significance of this study lies in enhancing the comprehensive performance of PC beam structures, thus broadening its utilization scope within structural engineering.