Ultrathin β -MnOOH nanofi bers can be produced on a large scale via a greenchemical method using an aqueous solution of very dilute Mn(NO 3 ) 2 and aminoethanol at room temperature. High-magnifi cation electron microscopy demonstrates that the β -MnOOH nanofi bers are 3-5 nm thin and up to 1 micrometer long and the nanofi bers are parallel assembled into bundles with an average diameter of 25 nm. By a fi ltration process, ultrathin mesoporous membranes with strong mechanical, thermal, and chemical stabilities are prepared from the β -MnOOH nanofi ber bundles. The membranes can separate 10-nm nanoparticles from water at a fl ux of 15120 L m − 2 · h − 1 · bar − 1 , which was 2-3 times higher than that of commercial membranes with similar rejection properties. Based on the Young-Laplace equation, β -MnOOH nanofi ber/ polydimethylsiloxane composite membranes are developed through a novel downstream-side evaporation process. From nanoporous to dense separation membranes can be achieved by optimizing the experimental conditions. The membranes show desirable separation performance for proteins, ethanol/ water mixtures, and gases. The synthesis method of β -MnOOH nanofi bers is simple and environmentally friendly, and it is easily scalable for industry and applicable to other metal oxide systems. These composite membranes constitute a signifi cant contribution to advanced separation technology.