Tuning interactions at the interfaces in carbon fiber (CF)-reinforced polymer composites necessitates the implementation of CF surface modification strategies that often require destructive environmentally unfriendly chemistries. In this study, interfacial interactions in cellulose-based composites are tailored by means of a mussel-inspired adhesive polydopamine (PDA) coating, being inherently benign for the environment and for the structure of CFs. The step-by-step growth of PDA was followed by increasing treatment time leading to a hydrophilic PDA-coated surface, presumably via surface-based polymerization mechanisms attributed to strong π−π stacking interactions. Although PDA deposition led to an initial increase in the interfacial shear strength (IFSS) (5 h), it decreased at a longer reaction time (24 h), the formation of weakly attached PDA particles on the coated surface can possibly lie behind the latter phenomenon. Nevertheless, the mechanical properties of the prepared short CF-reinforced composite were improved (tensile strength increased ∼12% compared to the unmodified surface) with decreasing IFSS owing to the particular morphological design, resulting in longer fiber segments. Our study underlines the importance of the morphological design at the interface and considers PDA as a promising bioinspired material to tailor interfacial interactions.