LAUSR

Robust neuromorphic computing in the Big Data era calls for long‐term stable crossbar‐array memory cells; however, the elemental segregation in the switch unit and memory unit that inevitably occurs upon cycling breaks the compositional and structural stability, making the whole memory cell a failure. Searching for a novel material without segregation that can be used for both switch and memory units is the major concern to fabricate robust and reliable nonvolatile cross‐array memory cells. Tellurium (Te) is found recently to be the only peculiar material without segregation for switching, but the memory function has not been demonstrated yet. Herein, apparent piezoelectricity is experimentally confirmed with spontaneous polarization behaviors in elementary 2D Te, even in monolayer tellurene (0.4 nm), due to the highly oriented polarization of the molecular structure and the non‐centrosymmetric lattice structure. A large memory window of 7000, a low working voltage of 2 V, and high on switching current up to 36.6 µA µm−1 are achieved in the as‐fabricated Te‐based memory device, revealing the great promise of Te for both switching and memory units in one cell without segregation. The piezoelectric Te with spontaneous polarization provides a platform to build robust, reliable, and high‐density logic‐in‐memory chips in neuromorphic computing.