Herein, we report the synthesis of Cu-Ca-Al/NO3-based layered double hydroxide through co-precipitation methodology. The prepared layered double hydroxide was then modified with itaconic acid. The physicochemical properties of the prepared materials were studied using Fourier transform-infrared spectroscopy, scanning electron microscopy, X-ray diffraction analysis, thermogravimetric analysis, and nitrogen adsorption/desorption technique. The prepared materials were then applied as novel adsorbents for the removal of Congo red as a model of an anionic dye from aqueous media. To reach maximum adsorption, the effect of parameters including sample solution pH, adsorbent amount, contact time, and initial concentration of Congo red on the adsorption process was investigated. Kinetic studies were also conducted to study the mechanism of adsorption. In this regard, the kinetic models of pseudo-first-order, pseudo-second-order, Elovich, and intra-particle diffusion were studied. The results showed that the adsorption of Congo red onto Cu-Ca-Al-LDH and LDH-ITA adsorbents followed the pseudo-second-order kinetic model. To evaluate the equilibrium adsorption data, different isotherms including Langmuir, Freundlich, and Dubinin-Radushkevich were also applied. The data revealed that the Freundlich isotherm provided the best fit with the equilibrium data of both adsorbents. Maximum adsorption capacities of 81 and 84 mg g− 1 were obtained using Cu-Ca-Al-LDH and LDH-ITA adsorbents, respectively.