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In this study, high-purity cellulose nanofibrils (CNFs) were environmentally friendly extracted from natural bamboo. Physical, chemical, and mechanical treatments were comprehensively investigated, and then ensembled to effectively and efficiently remove lignin and hemicellulose with low energy from raw bamboo fibers, which combine microwave liquefaction, hydrogen peroxide-acetic acid delignification, alkaline treatment, and along with acid hydrolysis. This was able to allow for the extraction of CNFs. Compositional analysis, Fourier-transform infrared spectroscopy, X-ray diffraction, X-ray photoelectron spectroscopy, and thermogravimetric analysis were performed to investigate and confirm the successful removal of undesirable lignin and hemicellulose. The resultant cellulose fibers were then subjected to a mechanical treatment to obtain the cellulose nanofibrils. It was found that the obtained CNFs have an average diameter of 13 nm with a cellulose purity of 94.52%. Without any further surface modification, the incorporation of bamboo-based CNFs into natural rubber (NR) exhibits significant improvement in their mechanical properties including modulus (~66.67%), tensile strength (~120.83%), toughness (~139.34%), and elongation at break (~31.41%). Interestingly, there is no compromise between tensile strength and elongation at break for the nanocomposites. DMA results also showed that both storage and loss moduli were dramatically enhanced over those of neat NR in their glassy region, which is typically unusual. This study can show, if optimized for material extraction, the great promise to the potential use of natural materials to develop environmentally friendly composites with multi-functionality in a variety of real-world engineering structural applications. [ABSTRACT FROM AUTHOR]