In this study, we report the isolation of cellulose nanocrystals (CNCs) from Isora plant fibers by sulfuric acid hydrolysis and their assembly on hydrophilic cellulose and silicon-di-oxide (SiO2) surfaces via a layer-by-layer (LBL) deposition method. The isolated CNCs were monodispersed and exhibited a length of 200–300 nm and a diameter of 10–20 nm, a negative zetapotential (–34–39 mV) over a wide pH range, and high stability in water at various concentrations. The multi-layered structure, adsorbed mass, conformational changes, and anticoagulant activity of sequentially deposited anionic (sulfated) CNCs and cationic polyethyleneimine (PEI) on the surfaces of cellulose and SiO2 by LBL deposition were investigated using a quartz crystal microbalance technique. The organization and surface features (i.e., morphology, thickness, wettability) of CNCs adsorbed on the surfaces of PEI deposited at different ionic strengths (50–300 mM) of sodium chloride were analysed in detail by profilometry layer-thickness, atomic force microscopy and contact angle measurements. Compared to cellulose (control sample), the total coagulation time and plasma deposition were increased and decreased, respectively, for multilayers of PEI/CNCs. This study should provide new possibilities to fabricate and tailor the physicochemical properties of multilayer films from polysaccharide-based nanocrystals for various biomedical applications.

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