This study proposed a novel and low-cost adsorbent prepared from dredging sediment (DSD) for effective removal of dye in aqueous solutions. The adsorption efficiency and behavior of the DSD adsorbent toward the crystal violet (CV), a cationic dye, were investigated via batch experiments. The results showed that DSD samples contain mainly clay minerals (illite and kaolinite) and other mineral phases. In addition, DSD is a mesoporous material (Vmesopore = 94.4%), and it exhibits a relatively high surface area (~39.1 m2/g). Adsorption experiments showed that the solution’s pH slightly affects the adsorption process, and a pH of 11 gave a maximum capacity of 27.2 mg/g. The kinetic data of CV dye adsorption is well described by the pseudo–second-order and the Avrami models. The Langmuir and Liu isotherm models provide the best fit for the adsorption equilibrium data. The monolayer adsorption capacity of Langmuir reached 183.6, 198.0, and 243.6 mg/g at 293, 308, and 323 K, respectively. It was also found that the adsorption process was spontaneous (−ΔG°), exothermic (−∆H°), and increased the randomness (+∆S°) during the adsorption operation. The primary mechanisms in CV dye adsorption were ion exchange and pore filling, whereas electrostatic attraction was a minor contribution. In addition, three steps involving intraparticle diffusion occur at the same time to control the adsorption process. The results of this study highlight the excellent efficiency of DSD material as an ecofriendly sorbent for toxic dyes from water media.