Metal oxoanions, mostly toxic and polluting, are challenging to remove in complicated natural environments due to their specific ionic structures and electrical properties. Although many efforts have been developed to sequester metal oxoanions, traditional adsorption materials suffer from poor selectivity and instability. Covalent organic frameworks (COFs), known for their robust stability and customizable structures, have emerged as promising candidates for the removal of metal oxoanions. This review highlights recent advances in the use of COFs and similar materials for metal oxoanion sequestration. It also discusses various strategies to enhance the adsorption performance and selectivity of COFs, such as structural design and post‐synthetic modifications. Additionally, current challenges and future directions for improving the efficiency of COFs in metal oxoanion sequestration are summarized.