Cellulose nanofibrils (CNF) functionalized by introduction of trimethylammonium chloride were investigated for the uptake of arsenate [As(V)] from aqueous solutions. The modified-CNF was characterized using Energy Dispersive Spectrometry (EDS), argentometric titration, Boehr titration, zeta-potential, Scanning Electron Microscopy (SEM), Fourier Transform Infrared (FTIR) spectroscopy, Nuclear Magnetic Resonance (NMR) spectroscopy, Brunauer-Emmet-Teller (BET), and Dynamic Light Scattering (DLS). The modified-CNF was effective for As(V) removal from laboratory and field samples. The As(V) adsorption was rapid and equilibrium was attained within two hours. The kinetic data were adequately described by the pseudo-second-order kinetics model suggesting that As(V) adsorption onto modified-CNF involves electrostatic forces and bonds between As(V) and adsorption sites. The adsorption isotherm data were well correlated with model. The modified-CNF exhibited an As (V) adsorption capacity (q(e)) of approximately 25.5 mg g(-1). Competitive adsorption between As(V) and anions including NO2-, NO3-, and SO42- was investigated and the results showed negligible influence on As(V) removal. However, PO43- presence slightly reduced As(V) adsorption. Thermodynamics study showed that the As(V) adsorption onto modified-CNF is temperature dependent and is spontaneous and exothermic. Overall, the results of this study demonstrated that modified-CNF offers a propitious alterative for As(V) removal from water.