This study demonstrates the ecofriendly synthesis of iron-oxide nanoparticles (IONPs) and their stabilization with polymers, i.e., chitosan (C) and polyvinyl alcohol (PVA)-alginate (PA), along with a further investigation for the removal of arsenic(As(V)) from water. IONPs with an average diameter of less than 100 nm were prepared via a green synthesis process using an aqueous leaf extract of Terminalia chebula. Batch experiments were conducted to compare the removal efficiency of As(V) by these adsorbents. Factors such as pH and adsorbent dosages significantly affected the removal of arsenate As(V) by IONPs and polymer-supported reactive IONPs. Several adsorption kinetic models, such as pseudo first-order, and pseudo second-order Langmuir and Freundlich isotherms, were used to describe the adsorption of As(V). The removal of As(V) by IONPs follows the Langmuir adsorption isotherm. The highest monolayer saturation adsorption capacity as obtained from the Langmuir adsorption isotherm for IONPs was 28.57 mg/g. As(V) adsorption by polymer-supported IONPs best fit the Freundlich model, and maximum adsorption capacities of 34.4 mg/g and 40.3 mg/g were achieved for chitosan-and PVA-alginate-supported IONPs, respectively. However, among these absorbents, PVA-alginate-supported IONPs were found to be more effective than the other adsorbents in terms of adsorption, stability, and reusability.Among the various water treatment technologies, adsorption seems to be a more convenient and effective method for the removal of heavy metals in terms of cost and simplicity of process [10]. Iron and related adsorbents are popular for the remediation of water pollutants [11]. The intervention of nanotechnology opened a new horizon in the field of water purification [12]. Iron nanoparticles (NPs), which possess a high surface area and surface reactivity, are effectively used for water treatment [13,14]. Zero-valent iron nanoparticles (nZVIs) and iron oxide nanoparticles, such as Fe 2 O 3 and Fe 3 O 4 NPs, are among those commonly employed for the remediation of environmental pollution, particularly for the decontamination of water [15][16][17][18]. Magnetic nanoparticles and modified magnetic nanoparticles were found to be very effective for the removal of arsenic because of their strong adsorption activities, and they can be easily separated by employing an external magnetic field [19][20][21]. Evidence of the particle size influence on the ability to remove (adsorb) arsenic from water was observed, as smaller nanoparticles were found to exhibit more adsorption capacity and faster kinetics due to their higher specific surface area, shorter intraparticle diffusion distance, and larger number of surface reaction sites of nanoparticles [22,23]. The nanopowder form of metal oxides/hydroxides provides a high surface area for increased adsorption capacity; however, this small particle size also drives the need for energy-intensive post-treatment filtration to recover the nanoparticles for regeneration and reuse [24]. To overcome this issue,...