Biological structures ranging in size from molecules to organelles, cells, organs, tissues, and the human body are exquisitely structured in three-dimensions (3D). In order to mimic, sense, or to interface functional devices with biological ones, there is a need to create 3D, artificially structured materials or 3D, heterogeneously integrated, functional devices (from nano- to macro- scales). Existing conventional fabrication/assembly technologies have facilitated the representation of 2D networks of interface active devices or platform with biology, but the technology is impeded in its application to complex 3D geometries that requires hierarchical precision and multi-material heterogeneity. The solutions generally require fundamental, conceptual advances in materials science and engineering. A number of strategies have been developed to overcome these obstacles but have not been entirely successful. Our approach is to use bioprinting and origami-inspired self-folding, which are advanced manufacturing technologies that permit the manufacturing of complex multi-material, multi-scale, and/or multi-functional 3D devices. Toward this end, our research aims at developing a smart platform of 3D advanced functional devices for diverse applications in 3D biomedical devices and nano-electronic devices, opening new opportunities to test therapeutic options.