focused on stretchable electronic devices, including photovoltaic devices, [4] lightemitting devices, [5] sensors, [6] and transistors. [7][8][9] Currently, two main strategies are used to produce stretchable devices. The first involves transforming the geometry of conventional brittle materials into mesh, [10] serpentine, [11] crack, [12] and longitudinal wave [13] structures, which reduces the deformation of the active material. Another approach is to produce intrinsically stretchable materials. Intrinsically stretchable devices have been extensively researched because of their potential to produce low-cost, large-area, and highdensity devices, as well as their seamless integration into stretchable applications.To produce an intrinsically stretchable device, each component that makes up the device must be stretchable. One of the current challenges is to produce an intrinsically stretchable semiconductor layer because obtaining high charge transport properties requires crystalline or semi-crystalline polymers, while mechanical flexibility requires amorphous polymers. [14][15][16] Thus, a balance between crystalline and amorphous morphologies seems to be ideal for achieving stretchable semiconducting polymers. Semiconducting polymers with good mechanical and electrical properties can be obtained via molecular design and chemical synthesis, for example by main-chain engineering [17][18][19][20][21] and side-chain engineering. [22][23][24][25][26] In contrast to the complex chemical synthesis methods described above, the physical blending of polymeric semiconductors with insulating elastomers is a simple and effective way to obtain intrinsically stretchable semiconducting polymers. Due to the different solvent interaction parameter of the polymers, the blended polymers will phase separate, and the interpenetrating polymer networks will enhance the mechanical deformability due to the continuous film structure. [27][28][29][30][31][32] At the same time, the original semiconductor polymer acts as the charge transport material in a device, while the insulating polymeric elastomer provides the device with elasticity. Precise control of the film structure in the blend system may be an effective strategy to achieve intrinsically stretchable semiconducting poly mers. Poly-3-hexylthiophene (P3HT)/elastomer blends have been reported as a feasible approach to enhance Physically blending semiconducting conjugated polymers with elastomeric materials and precisely controlling the resulting film structure provides an effective strategy to obtain intrinsically stretchable semiconducting polymers. Here, vertically phase-separated ultrathin poly(3-hexylthiophene) (P3HT) and polystyrene-b-polyisoprene-b-polystyrene (SIS) blend films are developed for one-step fabrication of semiconductor and insulator layers of organic field effect transistors (OFETs). The phase-separated structure, surface morphology, and tensile deformation are characterized by UV-vis absorption spectroscopy, atomic force microscopy, and optical microscopy. The ble...