Surfaces are responsible for important interactions of biomaterials since they create the interface with the biological environment and affect the response that the body will have to the material. Surface roughness and morphology have great impact on the material performance, affecting cell, bacterial, and biomolecular adhesion. Thin films of chitosan and carboxymethyl cellulose were produced by layer-by-layer deposition at different pH values and had their surface growth process studied throughout roughness measurements. Both polymers are nontoxic and biocompatible to the human biological system, with biomedical applications from tissue engineering to drug delivery. Growth exponents are presented, and it is suggested that fractal-based growth models are suitable for describing surface evolution and morphology of carboxymethyl cellulose/chitosan layer-by-layer thin film growth during deposition, primarily nonlinear models.