The goal of this work was to design a new nanocarrier composed of the glycosaminoglycan hyaluronan and the polysaccharide chitosan, intended for the transmucosal delivery of macromolecules. The nanoparticles were characterized for their size and superficial charge. The incorporation of hyaluronan was verified by agarose gel electrophoresis and Fourier transform infrared (FT-IR) spectroscopy. The ability of the nanosystems to encapsulate macromolecules was studied taking the hydrophilic protein bovine serum albumin (BSA) and the hydrophobic polypeptide Cyclosporine A (CyA) as models. Results showed that the experimental conditions could be conveniently adjusted in order to modulate the physicochemical properties of the carriers and their composition. Moreover, the nanoparticles provided high association efficiencies of the selected macromolecules.