Arsenic is highly toxic, affecting millions of people in many regions of the world. That is why developing economic and efficient technologies is imperative to eliminate it. Sorption techniques are attractive as efficient and inexpensive sorbents can be used. Chitosan is an abundant, naturally occurring, biodegradable, low-cost biopolymer that can be combined with metal oxide to enhance its removability. This work aimed to synthesize a new chitosan–magnetite-based sorbent for arsenic removal. The synthesized sorbent does not present pores, and when using FT-IR, functional groups of the chitosan and the presence of As(V) in the sorbent treated with arsenic were identified. The synthesized magnetite was characterized using XRD spectroscopy. Application of the central composite design model showed that 0.22 g of the sorbent at pH 6.0 could remove 27.6% of As(V). Kinetic data, fitted with the pseudo-first and -second order models, indicated an ion exchange sorption and activation energy of 28.1–31.4 kJ mol−1. The isotherms were fitted with the Langmuir model, indicating favorable monolayer adsorption with high affinity. The sorption energy calculated using Dubinin Radushkevich, 9.60–8.80 kJ mol−1, confirms a sorption mechanism mediated by ion exchange. The thermodynamic parameters of the process were ΔG° (−21.7/−19.7 kJ mol−1), ΔH°(16.7 kJ mol−1) and ΔS°(123.3 J mol−1 K−1).