The pollution of aquatic environments is a growing problem linked to population growth and intense anthropogenic activities. Because of their potential impact on human health and the environment, special attention is paid to contaminants of emerging concern, namely heavy metals. Thus, this work proposes the use of naturally derived materials capable of adsorbing chromium (VI) (Cr(VI)), a contaminant known for its potential toxicity and carcinogenic effects, providing a sustainable alternative for water remediation. For this purpose, membranes based on chitosan (CS) and chitosan/Kraft lignin (CS/KL) with different percentages of lignin (0.01 and 0.05 g) were developed using the solvent casting technique. The introduction of lignin imparts mechanical strength and reduces swelling in pristine chitosan. The CS and CS/0.01 KL membranes performed excellently, removing Cr(VI) at an initial 5 mg/L concentration. After 5 h of contact time, they showed about 100% removal. The adsorption process was analyzed using the pseudo-first-order model, and the interaction between the polymer matrix and the contaminant was attributed to electrostatic interactions. Therefore, CS and CS/KL membranes could be low-cost and efficient adsorbents for heavy metals in wastewater treatment applications.