Water-purifying materials are of vital importance for providing sanitary water, especially in epidemic and disaster areas and for wilderness survival. Here, we report a novel inorganic composite with a fast, reusable, and pleiotropic water purification ability. The composite of heterogeneous Ni−La 2 O 3 nanofibers was developed using an easy, low-cost, and large-scale production process, i.e., an electrospinning technique. Because of the unique heterostructure formed by introducing nickel nanoparticles into the La 2 O 3 host, the nanocomposite fibers can rapidly remove various detrimental micropollutants with absorption rate constants hundreds of times greater than those of inorganic materials and activated carbons. In addition, the nanocomposite can be recycled by a soft washing procedure at ambient temperature and demonstrates a much more stable performance than the state-of-the-art activated carbon materials. Furthermore, the nanofibers have an excellent germicidal effect against the high-risk human pathogen Escherichia coli. Our work introduces a promising inorganic absorbent suitable for purifying life-sustaining water supplies in emergency situations and alleviating worldwide water shortages.