In this work, Schiff base network-1 (SNW-1), as a new generation of covalent organic frameworks (COFs), was synthesized and modified by fabrication of a composite with clay mineral montomorillonite (Mt). It was used for simultaneous removal of anionic and cationic dyes from aqueous solutions. The fabricated composite was characterized successfully with various techniques. Tartrazine (TT) and methylene blue (MB) were selected as model anionic and cationic dyes, respectively. The effects of the percentage of each component in the composite, initial pH, and initial dye concentration were evaluated on the adsorption capacity. Adsorption reaction models and adsorption diffusion models were used to study the kinetic process of adsorption. Adsorption of both dyes reached equilibrium after 40 min. The obtained results were fitted to Langmuir, Freundlich, Temkin, and Dubinin-Radushkevich (D-R) models to predict the isotherms of adsorption. Under optimum conditions for removal of each dye with the composite, the maximum adsorption capacity of 519.2 and 602.7 mg g −1 were obtained for TT and MB, respectively. The used SNW-1/Mt composite could be regenerated by salty methanol. The high adsorption capacity and excellent reusability make SNW-1/Mt composite attractive for the simultaneous removal of anionic and cationic dyes from aqueous solutions.