Development of novel bio-based nanocomposites is fundamental to decrease the dependence on fossil resources in order to offer a sustainable future. The objective of this study was to synthesize and characterize cellulose nanoparticles from Enset ventricosum fibers. These fibers are one of the agricultural residues which are found in abundance, relatively inexpensive, and readily present as an available source of renewable lignocellulosic biomass. In the present study, cellulose was extracted from the Enset ventricosum fibers by a series of chlorination, alkaline extraction, and bleaching processes. This was followed by the synthesis of cellulose nanocrystal via H2SO4 hydrolysis, alkaline treatment, and bleaching with acidified sodium chlorite. Cellulose extraction parameters were optimized using response surface methodology (RSM) with Design-Expert (R) Version-11 software, and the cellulose produced was characterized using Fourier transform infrared spectroscopy (FT-IR), X-ray diffraction (XRD), thermogravimetric analysis (TGA), and scanning electron microscopy (SEM). The Enset cellulose nanoparticle yield from Enset ventricosum was found to be 39.68\% at 50 degrees C, 45 min, and 55\% acid concentration. The Enset cellulose nanoparticle was characterized using FT-IR, SEM, and dynamic light scattering (DLS), and the particle size distribution and crystallinity were measured. The maximum particle size distribution of E-CNp based on the dynamic light scattering study was found to be of 91.5 nm. The peak observed around 898 cm(-1) in the FT-IR spectrum of extracted cellulose and treated nanocellulose was associated with the cellulosic beta-glyosidic linkages, and this indicated the stability of the cellulose molecular structure despite the chemical treatment of Enset fibers. SEM images of the E-CNp crystals showed a distinct morphology and size. The percentage crystallinity of the raw Enset fiber, cellulose, and E-CNp was found to be 48.12\%, 59.75\%, and 63.31\% respectively based on the XRD analysis. The crystallinity of E-CNp improved as the hydronium ions (H3O+) penetrated into the amorphous regions of cellulose components breaking beta-1,4-glycosidic linkages in the cellulose chains and thereby brought about the release of individual crystallites. TGA analysis indicated a decrease in the quantity of lignin and hemicellulose in the alkali-treated fibers, Enset cellulose, and E-CNp, compared to Enset fibers. The E-CNp was then used in the fabrication of Enset cellulose nanocomposite (E-CNc). The highest tensile strength of 42.9 MPa was observed in E-CNc for the PVA/6\%NC blend. The uniform distribution of nanocellulose in the PVA matrix provided evidence for the fabrication of a new composite material from Enset fibers. Thus, this study proves to be one of the novel attempts towards the sustainable application of Enset fibers.