Over the past few decades, there has been an increasing interest in the fabrication of complex high-resolution three-dimensional (3D) architectures at micro/nanoscale. These architectures can be obtained through conventional microfabrication methods including photolithography, electron-beam lithography, femtosecond laser lithography, nanoimprint lithography, etc. However, the applications of these fabrication methods are limited by their high costs, the generation of various chemical wastes, and their insufficient ability to create high-aspect-ratio 3D structures. High-resolution 3D printing has recently emerged as a promising solution, as it is capable of building multifunctional 3D constructs with optimal properties. Here we present a review on the principles and the recent advances of high-resolution 3D printing techniques, including two-photon polymerization (TPP), projection microstereoLithography (PµSL), direct ink writing (DIW) and electrohydrodynamic printing (EHDP). We also highlight their typical applications in various fields such as metamaterials, energy storage, flexible electronics, microscale tissue engineering scaffolds and organ-on-chips. Finally, we discuss the challenge and perspective of these high-resolution 3D printing techniques in technical and application aspects. We believe that high-resolution 3D printing will eventually revolutionize the microfabrication processes of 3D architectures with high product quality and diversified materials. It will also find applications in a wide scope.

Electrohydrodynamic printing (EHDP), based on the electrohydrodynamically induced flow of materials, enables the production of micro/nanoscale fibers or droplets and has recently attracted extensive interest to fabricate user-specific patterns in a controlled and high-efficiency manner. However, most of the existing EHDP techniques can only print two-dimensional (2D) micropatterns which cannot meet the increasing demands for the direct fabrication of three-dimensional (3D) microdevices. The integration of EHDP techniques with the layer-by-layer stacking principle of additive manufacturing has emerged as a promising solution to this limitation. Here we present a state-of-the-art review on the translation of 2D EHDP technique into a viable micro/nanoscale 3D printing strategy. The working principle, essential components as well as critical process parameters for EHDP are discussed. We highlight recent explorations on both solution-based and melt-based 3D EHDP techniques in cone-jet and microdripping modes for the fabrication of multimaterial structures, microelectronics and biological constructs. Finally, we discuss the major challenges as well as possible solutions with regard to translating the 3D EHDP process into a real micro/nanoscale additive manufacturing strategy for the freeform fabrication of 3D structures.

Mimicking the hierarchical microarchitecture of native myocardium in vitro plays an important role in cardiac tissue engineering. Here we present a novel strategy to produce multiscale conductive scaffolds with layer-specific fiber orientations for cardiac regeneration by combining solution-based and melt-based electrohydrodynamic (EHD) printing techniques. Polycaprolactone (PCL) microfibers were printed by melt-based EHD printing and the fiber orientation was flexibly controlled in a layer-by-layer manner according to user-specific design. The as-printed microfibrous scaffolds can provide the seeded cells necessary contact cues to guide layer-specific cellular alignments. Sub-microscale conductive fibers were simultaneously incorporated inside the well-organized PCL scaffolds by solution-based EHD printing, which significantly improved the conductivity as well as the cellular adhesion and proliferation capacity. The multiscale conductive scaffolds can further direct the multiple-layer alignments of primary cardiomyocytes and facilitate cardiomyocyte-specific gene expressions, which exhibited enhanced synchronous beating behavior compared with pure microfibrous scaffolds. It is envisioned that the proposed hybrid EHD printing technique might provide a promising strategy to fabricate multifunctional micro/nanofibrous scaffolds with biomimetic architectures, electrical conductivity and even biosensing properties for the regeneration of electroactive tissues.

Additive manufacturing (AM) has drawn tremendous attention in various fields. In recent years, great efforts have been made to develop novel additive manufacturing processes such as micro-/nano-scale 3D printing, bioprinting, and 4D printing for the fabrication of complex 3D structures with high resolution, living components, and multimaterials. The development of advanced functional materials is important for the implementation of these novel additive manufacturing processes. Here, a state-of-the-art review on advanced material strategies for novel additive manufacturing processes is provided, mainly including conductive materials, biomaterials, and smart materials. The advantages, limitations, and future perspectives of these materials for additive manufacturing are discussed. It is believed that the innovations of material strategies in parallel with the evolution of additive manufacturing processes will provide numerous possibilities for the fabrication of complex smart constructs with multiple functions, which will significantly widen the application fields of next-generation additive manufacturing.