Adsorption-based atmospheric water harvesting (AWH) demonstrates innovative potential in mitigating global water scarcity through efficient vapor capture by means of adsorbent materials. Metal-organic frameworks (MOFs) are excellent water vapor adsorbents at low humidity. However, MOF as adsorbents in powder form often triggers agglomeration and limits practical application. It remains challenging to design robust materials for water harvesting to date. Here, we present a strategy to design bioinspired honeycomb-networked spindle-knotted water molecule capturing fiber mesh on large scale (i.e., BMCM), based on
MOFandthermo-responsive gel polymer using a biomimetic interfacial assembly method. The honeycomb-networked spindle knots ofBMCMachieveuniquecapabilitiesthatregulatethemorphologyofMOFnanocrystalstoexpandthewater-moleculesites andfavorwateruptake,alongwiththermo-responsiveswitchingbetweenwateruptake(e.g.,<30?C)andrelease(e.g.,>30?C).The
BMCMexhibitsthereby robust water uptake capabilities of ≈0.56–1.05 g g?1 at 30–80% relative humidity (RH), taking a short time rather thanothers. After reaching its saturation adsorption capacity at 30%RH,itcanrelease≈0.53gg?1 ofmoisturewithin30min
under one solar irradiation, with a water release capacity as high as 95%. As for BMCM on large scale outdoor, water production rate reaches ≈3.41 L/kg/day on average after 5-day cycles in atmospheric air condition. This study provides an insight into the
designing of next-generation AWH materials, which would be extended into applications, e.g., water engineering in industry, outdoor portable system or devices, etc.