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Significance Engineering multiple functions in a single material format is a key design parameter to fabricate devices that can perform at the confluence between biology and technology. This can be achieved by designing materials with hierarchical structures across several scales or by embedding active molecules at the point of material formation. These approaches have been successfully pursued to engineer 2D materials formats. However, current technologies have limited the formation of 3D constructs with orthogonal functions. In this study, we demonstrate an entirely water-based sol–gel–solid process to generate 3D mechanical forms that embed biological (and other) functions. This approach is a step toward the development of multifunctional devices that may liaise between the biotic and abiotic worlds.

Programming function into mechanical forms by directed assembly of silk bulk materials