The formation of a rigid tough interface based on a nacre-like structure in carbon fiber (CF) composites is a promising way to eliminate low delamination resistance. An effective method of coating CFs is electrophoretic deposition (EPD), which, in the case of dissimilar components like graphene oxide (GO) and polymeric glue, usually requires their chemical bonding/ strong interactions. In this work, we focus on chitin nanocrystals (ChNCs), leading to an excellent mechanical performance of artificial nacre, where favorable interactions and bonding with GO were controlled by degrees of deacetylation (5, 15 and 30 %). We have prepared coatings based on GO/ChNCs adducts with 95/5, 90/10,50/50 and 25/75 ratios using optimized EPD conditions (pH, concentration, voltage and time). The prepared materials were characterized using FTIR, TEM, XPS, SEM, DLS, and XRD. SEM evaluation indicates the formation of a homogeneous interlayer, which possesses a fair ability of chemical bonding with the epoxy matrix. Short beam testing of epoxy matrix composites indicates that coating does not decrease stiffness and its relatively low dependence on composition. Therefore, all coatings are promising for a detailed study of delamination resistance using laminate samples. Moreover, facile EPD from water solution/ suspension has a fair potential for industrial applications.