Herein, walnut shell (WS) was utilized as the raw material for the production of purified cellulose. The production technique involves multiple treatments, including alkaline treatment and bleaching. Furthermore, two nanocellulose materials were derived from WS by 2,2,6,6-tetramethylpiperidine-1-oxyl radical (TEMPO) oxidation and sulfuric acid hydrolysis, demonstrating the broad applicability and value of walnuts. The micromorphologies, crystalline structures, chemical functional groups, and thermal stabilities of the nanocellulose obtained via TEMPO oxidation and sulfuric acid hydrolysis (TNC and SNC, respectively) were comprehensively characterized. The TNC exhibited an irregular block structure, whereas the SNC was rectangular in shape, with a length of 55–82 nm and a width of 49–81 nm. These observations are expected to provide insight into the potential of utilizing WSs as the raw material for preparing nanocellulose, which could address the problems of the low-valued utilization of walnuts and pollution because of unused WSs.