Copper ions represent a critical water contaminant, posing substantial health and environmental hazards. Despite numerous efforts, a practical method to effectively eliminate such potentially toxic elements from aqueous solutions has remained elusive. Herein, we endeavor to fabricate and measure the ion adsorption performance of bio-based hydrogel nanocomposites composed of polyvinyl alcohol (PVA) and chitosan (CS) incorporated with hybrid carbon nanotube (CNT) and graphene (GNP). A well-dispersed microstructure is envisaged for single-particle and hybrid PVA/CS hydrogel nanocomposites, which are attributed to strong interactions between chemical moieties of components. Thermal analysis reveals the synergistic impact of nanoparticles on PVA/CS/CNT:GNP (1:3) and PVA/CS/CNT:GNP (1:1) specimens, indicating higher thermal stability of hydrogels with respective 9.13 and 4.8% compared to that pure hydrogel. The PVA/CS/CNT:GNP (1:3) sample showcases superior efficiency in copper ion removal at 27.17% and an adsorption capacity of 217.37 mg/g, which is roughly 54% higher than that of the pure PVA/CS hydrogel. The kinetic pseudo-second-order model with a correlation coefficient of 0.998 is aligned with the experimental data, confirming a well-suited description of the kinetics of copper ion adsorption by the hydrogels. Hence, the prepared hybrid PVA/CS hydrogel nanocomposites offer alluring candidates for ion removal applications from aqueous solutions.