Keywords: metal-organic frameworks • cellulose nanocrystals • aerogels • water purification • porous materialsThis work overcomes the longstanding challenge of processing metal-organic framework (MOF) powders into a convenient and tailorable form by entrapping them within a cellulose nanocrystal (CNC) aerogel. MOFs are a new class of porous materials, assembled from metal ions or ion clusters bridged by organic ligands. Since the pioneering work on MOF-5 reported by Yaghi and co-workers, [1] MOFs have received great attention due to their large surface area and porosity, high thermal stability, and tunable pore structure. MOFs have shown great potential in various applications including gas separation [2] and storage, [3] chemical sensing, [4] catalysis, [5] and so on. Designing and preparing new MOFs, [6] post-modification of existing MOFs, [7] and fabrication of MOFs into different structures [8] are currently of great interest.However, due to the crystalline nature of MOFs, they are most commonly found in powder form and their processability and handling remain a significant challenge. [9] Integrating MOFs onto or within various substrates to produce a shapeable, cost-efficient, and chemically inert product is one way to expand the potential applications of these functional materials.The deposition and growth of MOF particles on substrates has become a highly researched area but is severely constrained by the physical and chemical requirements of the substrate and gives materials with limited functionality. [10] Usually surface modifications are needed in Submitted to 2 order to increase the compatibility between MOFs and substrates, and while different methods to grow MOFs exist, including solvothermal, [11] secondary, [12] layer by layer growth, [13] and electrochemical deposition, [14] the substrates have to be stable during the process or restricted synthetic conditions must be employed. [15] Incorporation of MOF particles onto polymer or fiber substrates (of both synthetic [16] and natural origin [17] ), by blending, deposition or in situ growth, has been demonstrated. However, while these approaches overcome some of the disadvantages of preparing MOF-only materials or planar MOF films, most examples reported to date are either limited by low MOF loadings or reduced flexibility. [16b, 18] One alternative approach used to avoid processing or depositing MOFs is to produce metal organic framework gels (MOGs) which are high surface area MOF-like materials but they generally lack the ordered crystal lattice and desired physical properties of MOFs.[19]Nanocellulose shows great promise for use as a supporting substrate [20] or templating material [21] , especially in the form of cellulose aerogels and foams, because of its high strength, light weight, low cost, non-toxicity and its ability to be processed easily in water. [22] Cellulose nanocrystals (CNCs), cellulose nanofibrils (CNFs), and bacterial cellulose are the most common types of nanocellulose which are now being produced with con...