LAUSR

With the rapid development of two‐dimensional semiconductor technology, the inevitable chemical disorder at a typical metal–semiconductor interface has become an increasingly serious problem that degrades the performance of 2D semiconductor optoelectronic devices. Herein, defect‐free van der Waals contacts have been achieved by utilizing topological Bi2Se3 as the electrodes. Such clean and atomically sharp contacts avoid the consumption of photogenerated carriers at the interface, enabling a markedly boosted sensitivity as compared to counterpart devices with directly deposited metal electrodes. Typically, the device with 2D WSe2 channel realizes a high responsivity of 20.5 A W−1, an excellent detectivity of 2.18 × 1012 Jones, and a fast rise/decay time of 41.66/38.81 ms. Furthermore, high‐resolution visible‐light imaging capability of the WSe2 device is demonstrated, indicating its promising application prospect in future optoelectronic systems. More inspiringly, the topological electrodes are universally applicable to other 2D semiconductor channels, including WS2 and InSe, suggesting its broad applicability. These results open fascinating opportunities for the development of high‐performance electronics and optoelectronics.