Arsenic contamination is the most pressing issue for human health and the environment. Understanding its behavior and distribution in natural waters and developing potential materials for its removal plays a crucial role in tackling this problem. This review aims to present one of the most effective As removal methods: Metal–organic framework (MOF) and MOF-based materials (mMOF) adsorption and their integration into membranes. This study compiles the latest worldwide distribution of As in natural waters. Moreover, we indicate the optimal operational conditions and feasibility of the composites for As removal. This study provides a comprehensive report on the mechanism of As adsorption using MOFs, the development of mMOFs, and their integration into membranes to remove As species from a solution effectively. We also suggest perspectives on future research and development strategies for eco-friendly MOFs and mMOFs. Additionally, statistical methods are applied for the first time to evaluate their benefits compared with conventional adsorbents by considering multiple criteria that affect adsorption performance. Overall, mMOFs demonstrate more excellent properties than MOFs, such as high reusability and stability, short equilibrium time, applicability to removing both types of As, and remarkable interference tolerance. However, both MOFs and mMOFs are generally considered promising adsorbents over conventional adsorbents that can be effectively employed for practical water treatment applications by either adsorption or membrane processes in the near future.