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The development of cost-effective cellulose fibers by utilizing agricultural residues have been attracted by the scientific community in the past few years; however, a facile production route along with minimal processing steps and a significant reduction in harsh chemical use is still lacking. Here, we report a straightforward ultrasound-assisted method to extract cellulose nanofiber (CNF) from fibrous waste sugarcane bagasse. X-ray diffraction-based crystallinity calculation showed 25% increase in the crystallinity of the extracted CNF (61.1%) as compared to raw sugarcane bagasse (35.1%), which is coherent with Raman studies. Field emission scanning electron microscopy (FE-SEM) images revealed thread-like CNF structures. Furthermore, we prepared thin films of the CNF using hot press and solution casting method and compared their mechanical properties. Our experiments demonstrated that hot press is a more effective way to produce high strength CNF films; Young’s modulus of the thin films prepared from the hot press was ten times higher than the solution casting method. Our results suggest that a combination of ultrasound-based extraction and hot press-based film preparation is an efficient route of producing high strength CNF films.