A very intense study class of complex porous materials, metal–organic frameworks (MOFs), composed of diverse central metallic ions attached to organic linkers, was used in this study as adsorbant materials from wastewaters. Phosphonate MOFs were prepared by the reaction of divalent inorganic salts (CoSO₄·7H₂O, NiSO₄·6H₂O, CuSO₄·5H₂O,) with vinyl phosphonic acid in hydrothermal conditions, obtaining cobalt, nickel, and copper vinylphosphonate (CoVP, NiVP, and CuVP). During synthesis the experimental conditions were varied in terms of time, temperature, and pH. The synthesized materials were characterized by Fourier transform infrared, thermogravimetric analysis, scanning electron microscopy, and X‐ray crystallography. The efficiency of MOFs as adsorbents was investigated for diverse initial dye concentrations at different pH values and at three temperatures (25, 40, and 55°C). The synthesized materials presented good efficiency in the elimination of anionic as well as cationic type of dyes from aqueous solutions. The highest adsorption capacities were obtained working at optimum solution pH 4.2 for Acid Orange 7 and 10 for Basic Fuchsine, using 1 g/L of MOFs at room temperature (25°C). The adsorption capacities increase in the following order: CuVP < NiVP < CoVP.