A huge amount of textile dyes are released as industrial waste into the environment each year, which alters the water’s natural appearance and causes toxicity and carcinogenicity in the human body. Peanut husk is considered an agro-waste and contains many valuable compounds, such as cellulose. Different concentrations of cellulose were extracted from peanut husk and then loaded with bio-silver nanoparticles, which were fabricated using neem leaves (Azadirachta indica) as a reducing agent to form Ag-cellulose nanocomposites (Ag-Cell-NCMs). Different devices were used to characterize Ag-Cell-NCMs. The TEM images displayed that the size of Ag-Cell-NCMs ranged between 13.4 and 17.4 nm after dye adsorption. The Ag-Cell-NCMs were used to adsorb toxic dyes such as crystal violet (CV). Different parameters were applied, such as the ratio of cellulose to Ag-NPs, pH, contact time, adsorbent dose, dye concentration, and the temperature required to reach the optimization conditions to remove CV dye from the aqueous solution. Different kinetics and isotherm models were applied to the experimental data to explain the mechanism of the adsorption process. The adsorption of CV on Ag-Cell-NCMs follows the pseudo-second order, and the best-fit isotherm was the Langmuir isotherm. The new composite was tested for the possibility of dye desorption and ability to be reused several times, and we found that the new nanocomposite can be reused for multiple adsorptions and there is a possibility of dye desorption.