The applicability of advanced composite materials with hierarchical structure that conjugate metal–organic frameworks (MOFs) with macroporous materials is commonly limited by their inferior mechanical properties. Here, a universal green synthesis method for the in situ growth of MOF nanocrystals within wood substrates is introduced. Nucleation sites for different types of MOFs are readily created by a sodium hydroxide treatment, which is demonstrated to be broadly applicable to different wood species. The resulting MOF/wood composite exhibits hierarchical porosity with 130 times larger specific surface area compared to native wood. Assessment of the CO₂ adsorption capacity demonstrates the efficient utilization of the MOF loading along with similar adsorption ability to that of pure MOF. Compression and tensile tests reveal superior mechanical properties, which surpass those obtained for polymer substrates. The functionalization strategy offers a stable, sustainable, and scalable platform for the fabrication of multifunctional MOF/wood‐derived composites with potential applications in environmental‐ and energy‐related fields.

Besides classical utilization of wood and paper, lignocellulosic biomass has become increasingly important with regard to biorefinery, biofuel production and novel biomaterials. For these new applications the macromolecular assembly of cell walls is of utmost importance and therefore further insights into the arrangement of the molecules on the nanolevel have to be gained. Cell wall recalcitrance against enzymatic degradation is one of the key issues, since an efficient degradation of lignocellulosic plant material is probably the most crucial step in plant conversion to energy. A limiting factor for in-depth analysis is that high resolution characterization techniques provide structural but hardly chemical information (e.g. Transmission Electron Microscopy (TEM), Atomic Force Microscopy (AFM)), while chemical characterization leads to a disassembly of the cell wall components or does not reach the required nanoscale resolution (Fourier Tranform Infrared Spectroscopy (FT-IR), Raman Spectroscopy).

Metal-organic frameworks (MOFs) are among the most attractive functional porous materials. However, their processability and handling remains a substantial challenge because MOFs generally occur in powder form due to their crystalline nature. Combining MOFs and cellulose substrates to fabricate engineered materials offers an ideal solution to broaden their utilization as functional materials. MOF/cellulose composites further provide remarkable mechanical properties, tunable porosity, and accessible active sites of MOFs. In this review, we summarize current state-of-the-art fabrication routes for MOF/cellulose composites, with a specific focus on the unique potential of utilizing three-dimensional bio-based cellulosic scaffolds. We highlight their utilization as adsorbents in the gas and liquid phase, for antibacterial and protein immobilization, chemical sensors, electrical energy storage, and other emerging applications. In addition, we discuss current limitations and potential future research directions in the field of MOF/cellulose composites for advanced functional materials.

We compare functional NFC composites and wood derived scaffolds regarding mechanical performance, electric and magnetic properties as well as oil/water separation and heavy metal remediation.

Mechanically robust and renewable Janus wood membranes with capability for autonomous water transport show excellent fog-capturing efficiency.

Elegant design principles in biological materials such as stiffness gradients or sophisticated interfaces provide ingenious solutions for an efficient improvement of their mechanical properties. When materials such as wood are directly used in high‐performance applications, it is not possible to entirely profit from these optimizations because stiffness alterations and fiber alignment of the natural material are not designed for the desired application. In this work, wood is turned into a versatile engineering material by incorporating mechanical gradients and by locally adapting the fiber alignment, using a shaping mechanism enabled by reversible interlocks between wood cells. Delignification of the renewable resource wood, a subsequent topographic stacking of the cellulosic scaffolds, and a final densification allow fabrication of desired 3D shapes with tunable fiber architecture. Additionally, prior functionalization of the cellulose scaffolds allows for obtaining tunable functionality combined with mechanical gradients. Locally controllable elastic moduli between 5 and 35 GPa are obtained, inspired by the ability of trees to tailor their macro‐ and micro‐structure. The versatility of this approach has significant relevance in the emerging field of high‐performance materials from renewable resources.