Inorganic semiconductors are vital for a number of critical applications but are almost universally brittle. Here, we report the superplastic deformability of indium selenide (InSe). Bulk single-crystalline InSe can be compressed by orders of magnitude and morphed into a Möbius strip or a simple origami at room temperature. The exceptional plasticity of this two-dimensional van der Waals inorganic semiconductor is attributed to the interlayer gliding and cross-layer dislocation slip that are mediated by the long-range In-Se Coulomb interaction across the van der Waals gap and soft intralayer In-Se bonding. We propose a combinatory deformability indicator (Ξ) to prescreen candidate bulk semiconductors for use in next-generation deformable or flexible electronics.

Hetero‐shaped thermoelectric (TE) generators (TEGs) can power the sensors used in safety monitoring systems of undersea oil pipelines, but their development is greatly limited by the lack of materials with both good shape‐conformable ability and high TE performance. In this work, a new ductile inorganic TE material, Ag20S7Te3, with high TE performance is reported. At 300–600 K, Ag20S7Te3 crystallizes in a body‐centered cubic structure, in which S and Te atoms randomly occupy the (0, 0, 1) site. Due to the smaller generalized stacking fault energy in the (101¯)[010] slip system, Ag20S7Te3 shows better ductility than Ag2S, yielding excellent shape‐conformability. The high carrier mobility and low lattice thermal conductivity observed in Ag20S7Te3 result in a maximum dimensionless figure of merit (zT) of 0.80 at 600 K, which is comparable with the best commercial Bi2Te3‐based alloys. The prototype TEG consisting of 10 Ag20S7Te3 strips displays an open‐circuit voltage of 69.2 mV and a maximum power output of 17.1 µW under the temperature difference of 70 K. This study creates a new route toward hetero‐shaped TEG.