A polymer-enhanced bentonite-sand mixture has been widely used as a clay liner. This research focuses on the potential use of chitosan as a natural polymer mixed with bentonite as a clay liner base material. The bentonite used is a type of calcium bentonite, which is easily obtained in the market. Meanwhile, chitosan is produced from shrimp shell waste and is also easily available in the market. The process of mixing chitosan with a percentage of 2–6% of bentonite was carried out using a certain method, which is described in detail in the article. The materials’ physical, chemical, and engineering characteristics, such as Atterberg limits, permeability, and compressive strength, were examined after mixing. The results show that the mixing process was successful for the finding of minerals and functional groups based on the XRD and FTIR results. Promising results of the study include larger clusters, higher plasticity, decreased permeability, and higher compressive strengths of the mixtures after chitosan was added to bentonite.