Increased awareness of environmental pollution has changed focus to the use of biodegradable materials because they lack persistence in the environment. This article focused on the production of cellulose nanocrystals from Zhombwe, Neorautanenia brachypus (Harms) CA Sm. bagasse using steam explosion, alkaline treatment, bleaching, purification, and acid hydrolysis. The chemical composition after the treatments was determined using TAPPI standards. Further characterization was done using x‐ray Diffraction (XRD), differential scanning calorimetry (DSC), Fourier transform infrared spectroscopy (FTIR), and thermogravimetric analysis (TGA). The nanoscale dimensions and morphology of the extracted nanocrystals was determined through field emission scanning electron microscopy (FE‐SEM). FTIR spectroscopy and DSC confirmed the removal of noncellulosic compounds. XRD revealed that N. brachypus bagasse contained cellulose type I, which partly endured morphological change to polymorph II after purification and hydrolysis. FE‐SEM revealed elliptical to rod‐shaped structures after acid hydrolysis, which had a mean length and width of 1103 nm and 597 nm respectively. TAPPI tests revealed that successive chemical treatments increased crystallinity by 29.7%, enriched cellulose content by 74.2%, reduced lignin content by 21.7%, and reduced hemicellulose to less than 1%. The semicrystalline nature of the material produced in our work is a promising candidate for swelling hydrogel applications in areas such as wound dressing, heavy metal removal, controlled drug delivery, agriculture, and sanitary products. Future studies may focus on surface modification of nanocrystals to improve their thermal stability and therefore expand their range for potential industrial applications.