Chitosan/Hydroxyapatite composites, enriched with relatively active -NH2 and -OH groups, have emerged as promising adsorbents for heavy metal removal. In this study, we harnessed the potential of CS/HAP composites by developing monolithic PLA@CS/HAP filters utilizing 3D printing and freeze-drying techniques. These filters possess both macroscopic and microscopic porous structures, endowing them with exceptional capabilities for removing heavy metals from water. The adsorption properties of CS/HAP composites were explored by varying the dosage, duration, and initial concentrations of copper ions. The maximum adsorption capacity for Cu2+ was determined to be approximately 119+/−1 mg/g at the natural pH and 298 K. Notably, the monolithic PLA@CS/HAP filters demonstrated remarkable efficiency in the removal of copper ions, with 90% of copper ions effectively removed within a mere 2-h period in a cyclic adsorption experiment. Furthermore, the PLA@CS/HAP filters exhibited a robust dynamic Cu2+ removal capacity (80.8% or even better in less than 35 min) in a dynamic adsorption experiment. Importantly, all materials employed in this study were environmentally friendly. In summary, the PLA@CS/HAP filter offers advantages such as ease of preparation, eco-friendliness, versatility, and broad applicability in diverse wastewater treatment scenarios, thereby presenting a significant potential for practical implementation.