In this work, we present two novel nanostructured hybrid materials based on a chitin matrix loaded with increasing amounts of graphene oxide and reduced graphene oxide nanosheets (nGO and rGO, respectively). Both kinds of material (Chi:nGO and Chi:rGO) were studied using different spectroscopic and rheological techniques with the aim of understanding the interaction mechanism between chitin and nGO/rGO and explaining how the type of filler and its proportion affects its reinforcement. The production of these hybrids represents not only the obtention of low-cost materials with mechanical resistance but also a good opportunity for developing materials with several applications according to their composition. The nGO and rGO were characterised through FT-IR and ESR for the determination of the oxidation degree of each nanofiller. Then, the hybrids were spectroscopically analysed with FT-IR, ESR and SAXS which demonstrated that the components do not interact through covalent bonding and the nanosheets are well-dispersed among the chitin matrix. Finally, a rheological behavior assay was performed and its results were analysed in terms of G′ and η*. In short, all the results allowed us to conclude that nGO acts as a more efficient reinforcer than rGO due to the higher amount of hydrogen bonding established with chitin.