Monolithic adsorbent removal of fluoride from water is considered an effective and non-secondary pollution method. Here, a portable hydroxyl-functionalized coal gangue-based cordierite porous ceramic sheet (ACGC-Fe) is prepared by using coal gangue solid waste with a specific silicon-aluminum-rich composition ratio and a small amount of magnesium oxide as a raw material through powder compression molding and mild chemical modification. The prepared ACGC-Fe can be used to treat fluorine-containing wastewater and the maximum adsorption of fluorine can reach 18.69 mg g⁻¹. The Langmuir (Freundlich) adsorption isotherm model and pseudo-second-order kinetic model here provided a satisfactory description of the fluoride removal operating mechanism, and it is confirmed that the adsorption mechanism of ACGC-Fe is mainly attributed to the chemisorption of hydrogen bonds (with hydroxyl group) and ionic bonds (with metal), and physical adsorption based on cordierite porous ceramic pores. This research will provide a new idea for designing high-performance materials by mining and analyzing the composition and structure characteristics of coal gangue solid waste itself and broaden the application range of high-value-added coal gangue solid waste.