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This study investigated the effect of cetyltrimethylammonium bromide(CTAB) modification on Tenebrio molitorchitin and its ability to adsorb Reactive Black 5 (RB5) from aqueous solutions. BET technique was used to analyze the surface area and pore volume of modified and unmodified chitin samples. The results showed that CTAB modification increased chitin samples’ surface area and pore volume. The effect of pH on the adsorption of RB5 by chitin samples was also investigated. The results showed that the modified and unmodified chitin samples had the highest adsorption capacity at pH 2. It was investigated whether there was a significant difference in efficiency between isolated chitin and CTAB-modified chitin and the results showed that there was a difference between unmodified chitin and CTAB-modified chitin samples in terms of RB5 adsorption at pH 2 and CTAB-modified chitin was more successful as an adsorbent. The increase in RB5 adsorption efficiency with CTAB-modified chitin was attributed to changes in surface area and pore volume. The adsorption of RB5 dye with CTAB-modified chitin was investigated using several isotherm models, Elovich, Freundlich, Harkins–Jura, Jovanovic, and Langmuir. The results indicated that the Langmuir isotherm model provided a better explanation for RB5 adsorption compared to the other tested models. Moreover, the adsorption of RB5 on CTAB-modified chitin follows the order pseudo-second-order model and adsorption shows endothermic character.