Nanocomposite coatings are of great interest as barrier coatings since synergy effects between matrix and additive properties can be achieved. This, however, requires favorable additive-matrix interactions to provide a strong interphase (interface region). In this work we elucidate the properties of two environmentally benign nanocomposite coatings based on a waterborne acrylate formulation with additives from renewable sources, i.e. either cellulose nanocrystals, CNC; or, alternatively, cellulose nanofibrils, CNF. We focus on the corrosion protective properties of these coatings and discuss the reason why the nanocomposite with CNC displays favorable corrosion protection properties whereas that with CNF does not. To this end we utilized scanning electron microscopy, water contact angle measurement, Fourier transform infrared spectroscopy and electrochemical impedance spectroscopy techniques to investigate the microstructure, surface wetting, interactions between cellulosic materials and matrix as well as corrosion protective properties of both composite coatings.