The application of an oppositely charged dual polymer system is a promising approach to enhance paper strength. In this work, modified chitosan (MCN), a cationic polymer, and carboxymethyl cellulose (CMC), an anionic polymer, were used sequentially to improve paper strength. The adsorption of MCN on cellulose fibers was analyzed via polyelectrolyte titration. The formation of MCN/CMC complex in water and the deposition of this complex on silicon wafers were investigated by means of atomic force microscope and quasi-elastic light scattering techniques. The results showed that paper strength was enhanced slightly with a layer-by-layer assembly of the polymers. However, if the washing stage, which was required for layer-by-layer assembly, was eliminated, the MCN/CMC complex was deposited on fibers more efficiently, and the paper strength was improved more significantly. The significant improvement was attributed to the extra development of fiber bonding, confirmed further by scanning electron microscope observation of the bonding area of fibers treated with or without washing. However, the brightness of papers was somewhat decreased by the deposition of the complex on fibers. Higher paper strength also was achieved using rapid drying rather than air drying.