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Bath, BA2 7AY, UK Dr. RC Maher The Blackett Laboratory Imperial College London London, SW7 2BZ, UK Prof. F. Guitian Instituto de Ceramica de Galicia Universidad de Santiago de Compostela, Spain the previous layers. To address this challenge, in this work, we functionalize CMG with a responsive polymer (a branched copolymer surfactant, BCS) to create “responsive” sheets whose interactions in water can be regulated using an external stimulus, in this case pH.[12–16] Using this approach it is possible to formulate water-based inks with viscoelastic properties optimized to print self-supporting 3D structures through nozzles with diameters ranging from 500 down to 100 µm (Figure 1). Additional treatments can be used to manipulate the chemistry and microstructure of the printed parts opening new possibilities in a wide range of key technological areas from energy storage to thermal management, sensing or catalysis.[9, 11, 17] GO is an atomically thin layer of carbon covalently bonded to different oxygen functional groups remaining from the chemical process used to exfoliate graphite.[1] Hydroxyl and epoxy groups are distributed within the basal plane along with un-oxidized graphitic islands, and carboxylic groups on the edges.[1] These carboxylic groups remain deprotonated at basic pH (Figure 1 a).[18] BCS is a copolymer composed of two main domains: poly (methacrylic acid)(PMA) and polyethylene glycol (PEG), which are crosslinked with ethylene glycol dimethacrylate (EGDMA) to provide a branched architecture.[12, 13, 15, 16] Each polymer chain end contains 1-dodecanethiol (DDT), which offers multiple hydrophobic anchoring …