AbstractStrategic metals play an indispensable role in the related industries. Their extraction and recovery from water are of great significance due to both their rapid consumption and environmental concern. Biofibrous nanomaterials have shown great advantages in capturing metal ions from water. Recent progress in extraction of typical strategic metal ions such as noble metal ions, nuclear metal ions, and Li‐battery related metal ions is reviewed here using typical biological nanofibrils like cellulose nanofibrils, chitin nanofibrils, and protein nanofibrils, as well as their assembly forms like fibers, aerogels/hydrogels, and membranes. An overview of advances in material design and preparation, extraction mechanism, dynamics/thermodynamics, and performance improvement in the last decade is provided. And at last, we propose the current challenges and future perspectives for promoting biological nanofibrous materials toward extracting strategic metal ions in practical conditions of natural seawater, brine, and wastewater.