Cellulose nanocrystals have been evaluated as reinforcement material in polymeric matrices due to their potential to improve the mechanical, optical, and dielectric properties of these matrixes. This work describes how high pressure defibrillation and chemical purification affect the sludge fiber morphology from micro to nanoscale. Microscopy techniques and X-ray diffraction were used to study the structure and properties of the prepared nanofibers and composites. Microscopic studies showed that the used individualization processes lead to a unique morphology of interconnected web-like structure of sludge fibers. The nanofibers are bundles of cellulose fibers having widths (5 to 30 nm) and estimated lengths of several micrometers.