Globally, water contamination by heavy metals is a serious problem that affects the environment and human health. Adsorption is the most efficient way of water treatment for eliminating heavy metals. Various hydrogels have been prepared and used as adsorbents to remove heavy metals. By taking advantage of poly(vinyl alcohol) (PVA), chitosan (CS), cellulose (CE), and the process for physical crosslinking, we propose a simple method to prepare a PVA-CS/CE composite hydrogel adsorbent for the removal of Pb(II), Cd(II), Zn(II) and Co(II) from water. Structural analyses of the adsorbent were examined by Fourier transform infrared (FTIR) spectroscopy, scanning electron microscopy-energy dispersive X-ray (SEM-EDX) analysis, and X-ray diffraction (XRD). PVA-CS/CE hydrogel beads had a good spherical shape together with a robust structure and suitable functional groups for the adsorption of heavy metals. The effects of adsorption parameters such as pH, contact time, adsorbent dose, initial concentration of metal ions, and temperature on the adsorption capacity of PVA-CS/CE adsorbent were studied. The adsorption characteristics of PVA-CS/CE for heavy metals may be completely explained by pseudo-second-order adsorption and the Langmuir adsorption model. The removal efficiency of PVA-CS/CE adsorbent for Pb(II), Cd(II), Zn(II), and Co(II) was 99, 95, 92, and 84%, respectively, within 60 min. The heavy metal’s hydrated ionic radius may be crucial in determining the adsorption preference. After five consecutive adsorption–desorption cycles, the removal efficiency remained over 80%. As a result, the outstanding adsorption-desorption properties of PVA-CS/CE can potentially be extended to industrial wastewater for heavy metal ion removal.