Recently, environmental and ecological concerns have become a major issue owing to the shortage of resources, high cost, and so forth. In my research, I present an innovative, environmentally friendly, and economical way to prepare nanocellulose from grass wastes with a sodium hypochlorite (NaClO) solution of different concentrations (1–6% mol) at different times 10–80 min, washed with distilled water, and treated with ultrasonic waves. The optimum yield of the isolated cellulose was 95%, 90%, and 87% NaClO at 25 °C for 20 min and with NaOH and H2SO4 at 25 °C with 5% M, respectively. The obtained samples were characterized by dynamic light scattering (DLS), Fourier-transform infrared (FT-IR) spectroscopy, and X-ray diffraction (XRD). The effect of test temperature and reaction times on the crystallinity index (IC) of GNFC with different treated mediums was carried out and investigated. The IC was analyzed using the diffraction pattern and computed according to the Segal empirical method (method A), and the sum of the area under the crystalline adjusted peaks (method B) and their values proved that the effect of temperature is prominent. In both methods, GNFC/H2SO4 had the highest value followed by GNFC/NaOH, GNFC/NaClO and real sample nano fiber cellulose (RSNFC). The infrared spectral features showed no distinct changes of the four cellulose specimens at different conditions. The particle size distribution data proved that low acid concentration hydrolysis was not sufficient to obtain nano-sized cellulose particles. The Zeta potential was higher in accordance with (GNFC/H2SO4 > GNFC/NaOH > GNFC/NaClO), indicating the acid higher effect.