The α-chitin whiskers were prepared by acid hydrolysis of α-chitin from Parapenaeus longirostris shells from Moroccan local sources. A chitosan nanoscaffold in the form of a colloidal solution was obtained from the deacetylation of α-chitin whiskers under alkaline conditions. Chitosan-based nanoparticles were prepared through ionic cross-linking and gelation of chitosan by tripolyphosphate. The chemical structure and physicochemical properties of α-chitin whiskers, chitosan nanoparticles and chitosan nanoscaffold were characterized using Fourier transform infrared spectroscopy (FTIR), X-ray diffractometry (XRD) and transmission electron microscopy (TEM). The length of the as-prepared whiskers ranged between 90 and 620 nm, while the width ranged between 9 and 63 nm, with the average values being about 354 and 25 nm, respectively. The obtained chitosan nanoparticles were consistently spherical with an overall diameter of approximately 32 nm. Chitosan nanoscaffold possessed an interconnected pore network with an average pore size of 200 nm.