Traditional　nanofiltration　membranes　allow　high　rejection　of　low　molecular　weight　organic　matter,　yet　suffer　from　a　low　flux　and　a　high　operation　pressure,　and　they　pose　an　environmental　concern　because　they　are　made　of　petroleum-based　polymers.　Herein,　a　novel　environmentally　friendly　filter　membrane　for　ultrafast　molecular　separation　has　been　developed　using　natural　and　artificial　biomaterials　as　building　units.　Cellulose　micron　fibers,　a　natural　biopolymer,　serve　as　a　stable　substrate　for　the　growth　of　hydroxyapatite　(HAP)　nanowire　bunches,　which　are　the　main　inorganic　components　of　bones　and　teeth.　The　vertically　aligned　HAP　nanowire　bunches　provide　abundant　nanoscale　surfaces　and　confinement　space　for　the　attachment　of　dopamine　and　subsequently　self-polymerization　into　polydopamine　(PDA)　sub-micron　particles,　which　are　a　melanin-like　bioactive　polymer.　On　the　one　hand,　the　as-built　micro-nano　hierarchical　configuration　enables　ultrahigh　permeance　(＞6000　L　m−2　h−1　bar−1)　through　the　filter　membrane　at　a　low　pressure　(62　mbar).　On　the　other　hand,　molecular　dynamics　simulations　reveal　that　synergy　between　multiple　molecular　interactions　of　HAP　and　PDA　contributes　to　the　universal　separation　of　different　organic　pollutants　from　water　(i.e.,　cationic　and　anionic　dyes　and　antibiotics)　at　a　high　removal　rate　of　＞　97　%.　Overall,　this　work　ingeniously　uses　biocompatible　biomaterials　to　build　a　hierarchical　filter　membrane,　thereby　enabling　ultrafast　and　efficient　molecular　separation.　©　2024　Elsevier　B.V.