We propose a universal strategy to 3D printing the graphene oxide (GO) complex structure with GO highly aligned and densely compacted, by the combination of direct ink writing and constrained drying. The constraints not only allow the generation of a huge capillary force accompanied by water evaporation at nanoscale, which induces the high compaction and alignment of GO, but also limit the shrinkage of the extruded filaments only along the wall thickness direction, therefore, successfully maintaining the uniformity of the structure at macroscale. We discover that the shrinkage stress gradually increased during the drying process, with the maximum exceeding ∼0.74 MPa, significantly higher than other colloidal systems. Interestingly, because of the convergence between plates with different orientations of the constraints, a gradient of porosity naturally formed across the thickness direction at the corner. This allows us to 3D print humidity sensitive GO based soft robotics.
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