Direct Process‐Assembled Multidimensional Nanofiber Structures via Electrospinning

ABSTRACT Electrospun nanofibers possess exceptional structural characteristics, including well‐interconnected channels, nanoscale pore size, and high porosity, making them promising candidates for diverse applications across multiple fields. Structural design has emerged as a critical strategy for further enhancing the performance of these fiber materials. However, the inherent complexity of the electrohydrodynamic jet instability and solvent evaporation during electrospinning presents a significant challenge for rational fiber structure design. In this study, direct forming techniques are proposed to design the structures of fiber materials in three dimensions, encompassing the jet, fiber, and fiber assembly. Through regulating the spinning parameters, solvent systems, and electric field conditions, we successfully construct a garland‐like jet structure, wave‐like pure polymeric fiber morphology, and aligned fiber assembly. This work develops facile yet effective methods for the multi‐dimensional structural design of electrospun nanofibers, paving the way for the production of high‐performance and multifunctional fiber materials.