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Atomically thin materials, leveraging their low‐dimensional geometries and superior mechanical properties, are amenable to exquisite strain manipulation with a broad tunability inaccessible to bulk or thin‐film materials. Such capability offers unexplored possibilities for probing intriguing physics and materials science in the 2D limit as well as enabling unprecedented device applications. Here, the strain‐engineered anisotropic optical and electrical properties in solution‐grown, sub‐millimeter‐size 2D Te are systematically investigated through designing and introducing a controlled buckled geometry in its intriguing chiral‐chain lattice. The observed Raman spectra reveal anisotropic lattice vibrations under the corresponding straining conditions. The feasibility of using buckled 2D Te for ultrastretchable strain sensors with a high gauge factor (≈380) is further explored. 2D Te is an emerging material boasting attractive characteristics for electronics, sensors, quantum devices, and optoelectronics. The results suggest the potential of 2D Te as a promising candidate for designing and implementing flexible and stretchable devices with strain‐engineered functionalities.