Chitosan (CS), a positively charged polysaccharide, and magnesium aluminum silicate (MAS), a negatively charged clay with silicate layers, can electrostatically interact to form nanocomposite films. In this study, CS-MAS nanocomposite films were evaluated for use in tablet film coating. Effects of CS-MAS ratio and coating level on water uptake and drug release from the coated tablets were investigated. Surface and film matrix morphology of the coated film and the effect of enzymes in the simulated gastro-intestinal fluid on drug release were also examined. The results demonstrated that the CS-MAS coated tablets had a rough surface and a layered matrix film, whereas a smooth surface and dense matrix film on the CS coated tablets was found. However, the CS-MAS coated tablets provided fewer film defects than the CS coated tablets. Nanocomposite formation between CS and MAS could retard swelling and erosion of CS in the composite films in acidic medium. The higher MAS ratio of the CS-MAS coated tablets gave lower water uptake and slower drug release when compared with the CS coated tablets. Moreover, the CS-MAS films on the tablets presented good stability towards enzymatic degradation in simulated intestinal fluid. The release of drug from the CS-MAS coated tablets could be modulated by varying CS-MAS ratios and coating levels. Additionally, drug solubility also influenced drug release characteristics of the CS-MAS coated tablets. These findings suggest that the CS-MAS nanocomposites displays a strong potential for use in tablet film coating intended for modifying drug release from tablets.