In this work, Keggin type phosphomolybdate inorganic‐organic hybrid material coordinated to with iron was synthesized by hydrothermal process followed by precipitation with organic cation. The prepared hybrid was fully characterized using conventional spectroscopic techniques. The adsorption efficiencies of the hybrid were evaluated for the removal of both anionic and cationic dyes from aqueous solutions. From the studies, it was concluded that hybrid has high adsorption as well as high selectivity for anionic dyes than cationic dyes. The results from the adsorption experiments revealed that the hybrid have specific methyl orange dye removal efficiency ≥96 % for 20 mgL−1 concentration. The reaction kinetics and adsorption isotherm also discussed. [ABSTRACT FROM AUTHOR]