The scarcity of clean water has become a global environmental problem which constrains the development of public health, economy, and sustainability. In recent years, natural polyphenols have drawn increasing interests as promising platforms towards diverse water remediation composites and devices, owing to their abundant and renewable resource in nature, highly active surface chemistry, and multifunctionality. This review aims to summarize the most recent advances and highlights of natural polyphenol-based composite materials (e.g., nanofibers, membranes, particles, and hydrogels) for water remediation, by focusing on their structural and functional features, as well as their diversified applications including membrane filtration, solar distillation, adsorption, advanced oxidation processes, and disinfection. Finally, the future challenges in this field are also prospected. It is anticipated that this review will provide new opportunities towards the future development of natural polyphenols and other kinds of naturally occurring molecules in water purification applications.