In daily life, a large amount of dye-wastewater discharged poses a significant threat to the aqueous environment and human health due to its toxicity and even carcinogenicity.1 Therefore, the removal of these dyes is extremely important, but it will be more attractive if the recovery and recycling of raw materials can be realized at the same time, which is considerably challenging. In this regard, a lowcost and eco-friendly adsorption technology was considered to be more competitive2,3 than some other methods such as photocatalytic degradation, and so on.4,5 Activated carbon, as a traditional adsorbent in the treatment of dye-wastewater, is only effective for wastewater containing low concentrations of dye,6 and it has poor dye specificity due to its neutral framework. Thus, it is necessary to find a desirable adsorption material, which not only is able to reduce the pollutant organic dyes with high efficiency and low loss, but also realizes selective separation and recovery of raw materials. Polyoxometalates (POMs)-based organic–inorganic hybrid material may be a suitable choice. POMs, as an outstanding family of metaloxide clusters7,8 with controllable shape and size, highly electronegative, and oxo-enriched surfaces, are expected to exhibit good adsorption and selective separation towards cationic dyes because they may have a stronger attraction to cationic dyes than anionic dyes. Wang’s group recently reported a POM@MOF composite material, which demonstrates that various POMs incorporated into MIL-101 can improve the adsorption capacity for dyes.12 POMs-based hybrid materials as adsorption materials still have not been explored up to now, although they exhibit great potential for applications in various fields.9–11 With this in mind, we intend to design and synthesize novel POMs-based hybrid materials, and then further investigate their adsorption and regeneration behaviour for dye molecules from wastewater.