Pharmaceuticals are used to improve the lives of people across the globe. The high demand for their fabrication and use causes a very serious environmental threat since their presence is ubiquitous in aqueous matrices. For this reason, the synthesis, characterisation, and efficiency of three chitosan-based materials to eliminate pharmaceutical mixtures from aqueous solutions were examined in the present study. The target mixture comprised seven widely used drugs: carbamazepine, cyclophosphamide, adefovir, levofloxacin, metronidazole, glibenclamide, and trimethoprim. The grafting of poly(ethylene imine) and poly(acrylamide) on the chitosan structure allowed its physical characteristics to be controlled. An adsorption assessment was performed at different pH values, and it was concluded that pH = 4 was the optimum value. The adsorption kinetics revealed that the adsorption of a drug mixture involves a combination of physical and chemical adsorption. The adsorption process appeared to be finished after 1 h for all compounds of the studied mixture, with CS-AMI exhibiting the fastest kinetics. Mass adsorption experiments were also carried out to determine its effects. Overall, the grafting process significantly increased the adsorption capacity over the pristine material. Specifically, the highest capacity increase for CS-PEI was ~220% for carbamazepine, and for CS-AMI, it was 158% for trimethoprim. FT-IR, SEM, and XRD were used for the characterisation of the polymers. Based on the findings, the three materials are suggested as very effective adsorbents for the elimination of medicine residues from aqueous matrices.