vivo extracellular matrix (ECM). [2] Various advantages of the electrospun nanofiber membranes, including broad material selection, a high surface-area-to-volume ratio, controllability of physical properties (e.g., diameter and orientation of the nanofibers and porosity and thickness of the membrane), and capability in fabrication of complex nanostructures (e.g., coreshell and Janus nanofibers), [3] have made remarkable advancements in the development of in vitro tissue models and in vivo tissue regeneration. [1,2] Many studies have tried to control the spatial orientation of the electrospun nanofibers through electrospinning, given that the cellular activities, such as adhesion, migration, proliferation, and differentiation, could be promoted by the contact guidance through an anisotropic topographical cue of the electrospun nanofibers. Among various approaches to control the orientation of the electrospun nanofibers, including the electric fieldassisted method, rotating drum method, and magnetic electrospinning, [4-6] the electric field-assisted method readily modulates the orientation of the electrospun nanofibers in a precise and versatile manner. Based on the electric field-assisted method, previous studies have achieved various types of membranes from a uniaxially aligned nanofiber membrane to radially, circumferentially, and biaxially aligned nanofiber membranes, [6-8] showing their potential in manipulating many cell functions, such as myogenic differentiation of myoblast, dural fibroblast migration, and tight junction formation of endothelial cells. [9-11] However, the aligned nanofiber membrane produced by the electric field-assisted method is mechanically unstable, in general, because of its thin (<30 µm thick), anisotropic, and sparsely interconnected nanofibrous structures. [12-14] Hence, the aligned nanofiber membrane is prone to be damaged by external forces occurred with the experimental and surgical manipulations and the aqueous conditions during in vitro and in vivo biomedical applications. [9,15,16] An innovative approach to overcome such limitations of the aligned nanofiber membranes is to develop an electrospun bilayer membrane, also known as a kind of Janus sheet, composed of two membranes, one aligned and the other random, which simultaneously provide the anisotropic topographical Electrospun bilayer membranes comprising two layers, one aligned and the other random, have shown great potential in tissue engineering but previous fabrication processes inevitably relied on manual integration and produced limited types of membranes. Here, a metal-electrolyte solution dual-mode electrospinning (M-ELES) for fabrication of electrospun bilayer membrane based on a metal-electrolyte solution switchable collector is developed. The switchable collector enables random nanofiber deposition directly over the preexisting aligned nanofiber layer in an in situ manner and integration of the layers through an on-demand switch from the metal to the electrolyte solution collector. The electrolyte solution can eff...