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Processing metal-organic-frameworks (MOFs) into hierarchical macroscopic materials can greatly extend their practical applications. However, current strategies suffer from severe aggregation of MOFs and limited tuning of the hierarchical porous network. Here, we report a controlled strategy that can simultaneously tune the MOF loading, composition, spatial distribution, and confinement within various bio-originated macroscopic supports, as well as control the accessibility, robustness, and formability of the support itself. Our methodology enables the good dispersion of individual MOF nanoparticles on a spiderweb-like network within each macrovoid even at high loadings (up to 86 wt%), ensuring the foam pores are highly accessible for excellent adsorption and catalytic capacity. Additionally, this approach allows the direct pre-incorporation of other functional components into the framework. Our strategy provides a general toolbox for precise control over the properties of both the hierarchical support and MOF, opening new possibilities to construct tunable multi-scale porous platforms with desired functionalities. 

Various membranes have been developed for the separation of oil/water mixtures; however, their fabrication requires toxic reagents, multiple processing steps, and advanced technologies. Nature not only precisely generates unique materials but also provides tremendous examples in the environment that can be used as inspiration for the development and creation of smart and green materials. In this study, we prepare multifunctional nanobiofibers (NBFs) from grape seeds by a one-pot reaction using green solvents that, when made into a smart layer, can switch between a state of underwater superoleophobic wetting to a state of underoil superhydrophobicity and back without any external stimuli. The several μm length and 50 nm width NBFs exhibit robust stability and provide a porous NBF layer, suggesting their potential for the simultaneous separation of various surfactant-stabilized water-in-oil and oil-in-water emulsions while showing high dye adsorption from water (100% for methylene blue). Furthermore, by rolling water droplets on the surface of NBF powder, an effective microreactor, known as a liquid marble, is prepared for the first time using a bio-originated, superamphiphilic material in air, rather than hydrophilic or hydrophobic materials, and it can be used to remove dye within 30 s. Moreover, based on the ability of NBFs to encapsulate a high volume of water (120 μL), we demonstrate another application of the NBF powder as an additive to soil for maintaining soil moisture under arid conditions, allowing us to successfully demonstrate the growth of a lentil seed. This multi-functional, low-cost, and green NBF material shows excellent sustainability and mechanical/chemical stability for multiple promising environmental remediation applications.