Exfoliated bentonite sheets admixed with nano-cellulose fibers (EXB/CF) were prepared as advanced bio-composite of enhanced decontamination properties for different species of water pollutants (Cd2+, safranin dye, and phosphate). The composite achieved promising adsorption capacities with experimental values of 206.8 mg/g (Cd2+), 336 mg/g (safranin), and 296 mg/g (phosphate); and predicted maximum capacities of 212.9 mg/g (Cd2+), 341 mg/g (safranin), and 305 mg/g (phosphate). The adsorption systems for the three species follow the Freundlich isotherm model and Pseudo-First order as kinetic model considering both the linear and nonlinear fitting demonstrating heterogeneous and multilayer uptake properties of physisorption type. The operation of physisorption mechanisms was supported by the obtained adsorption energies from D-R model that are less than 8 kJ/mol as well as the calculated free energies and enthalpies. The thermodynamic investigation revealed the nature of the adsorption reactions of the three pollutants by EXB/CF as exothermic, favorable, and spontaneous reactions. The EXB/CF composite also is of significant recyclability value and applied in five decontamination reusing runs for Cd2+, safranin dye, and phosphate achieving promising removal percentages.