The impact of the ionic strength on the film growth has been studied for the architectures composed of chitin nanocrystals (ChiNC) and xyloglucan (XG) to better understand the fabrication process of multilayer films. The formation of ChiNC-XG assemblies was monitored by quartz crystal microbalance with dissipation (QCM-D) and multilayer films were fabricated by the spin-coating assisted layer-by-layer (LbL) procedure. Films were prepared from 1 g L-1 ChiNC dispersions at pH 4 without and with the addition of NaCl (0 and 5 mM, respectively) and 0.5 g L-1 XG solutions in water. Distinct growth pattern and structural characteristics were found for the films prepared from ChiNC at 0 and 5 mM NaCl. Specifically, films assembled without salt exhibited lower mass deposition and film growth failed after 5 (ChiNC-XG) bilayers. Differently, at 5 mM NaCl higher amounts of both polymers (ChiNC and XG) were adsorbed; therefore, the films were thicker, and the deposition succeeded up to 10 bilayers. Atomic force microscopy (AFM) revealed an almost completely covered surface after the adsorption of ChiNC at 5 mM NaCl whereas salt-free ChiNC dispersions resulted in lower surface coverage. These results reliably concluded that the fabrication of (ChiNC-XG) films requires the screening of the charges to promote the layers stability.