Materials coming from renewable resources have drawn recently an increased attention in various applications as an eco-friendly alternative in the synthesis of novel functional materials. Polysaccharides, with their prominent representative – chitosan (CS), are well-known for their sorption properties, being able to remove metal ions from dilute solutions either by electrostatic interactions or chelation. In this context, we proposed here a comparative study on Cu2+, Zn2+, Ni2+, Fe3+, and Cr3+ metal ions removal from industrial wastewaters by CS-based composite cryogels using batch technique. The composite cryogels consisting of CS embedding a natural zeolite, namely clinoptilolite, were synthesized by cryogelation, and their sorption performance were compared to those of CS cryogels and of acid-activated zeolite. A deeper analysis of thermodynamics and kinetics sorption data was performed to get insights into the sorption mechanism of all metal ions onto sorbents. Based on the optimized sorption conditions, the removal of the above-mentioned ions from aqueous solutions by the composite sorbent using dynamic technique was also evaluated.