AbstractTo deal with issues of process sustainability, cost, and efficiency, we developed materials reengineered from fibers to serve as super-bridging agents, adsorbents, and ballast media. These sustainable fiber-based materials considerably increased the floc size (~6,630 µm) compared to conventional physicochemical treatment using a coagulant and a flocculant (~520 µm). The materials also reduced coagulant usage (up to 40%) and flocculant usage (up to 60%). These materials could be used in synergy with coagulants and flocculants to improve settling in existing water treatment processes and allow facilities to reduce their capital and operating costs as well as their environmental footprint. Moreover, the super-sized flocs produced using fiber-based materials (up to ~13 times larger compared to conventional treatment) enabled easy floc removal by screening, eliminating the need for a settling tank, a large and costly process unit. The materials can be effective solutions at removing classical (e.g., natural organic matter (NOM) and phosphorus) and emerging contaminants (e.g., microplastics and nanoplastics). Due to their large size, Si- and Fe-grafted fiber-based materials can be easily recovered from sludge and reused multiple times.