LAUSR

Novel 2D semiconductors play an increasingly important role in modern nanoelectronics and optoelectronics. Herein, a novel topology designer based on component fusion is introduced, featured by the submolecular component integration and properties inheritance. As expected, a new air‐stable 2D semiconductor PdPSe with a tailored puckered structure is successfully designed and synthesized via this method. Notably, the monolayer of PdPSe is constructed by two sublayers via PP bonds, different from 2D typical transition metal materials with sandwich‐structured monolayers. With the expected orthorhombic symmetry and intralayer puckering, PdPSe displays a strong Raman anisotropy. The field‐effect transistors and photodetectors based on few‐layer PdPSe demonstrate good electronic properties with high carrier mobility of ≈35 cm2 V−1 s−1 and a high on/off ratio of 106, as well as excellent optoelectronic performance, including high photoresponsivity, photogain, and detectivity with values up to 1.06 × 105 A W−1, 2.47 × 107%, and 4.84 × 1010 Jones, respectively. These results make PdPSe a promising air‐stable 2D semiconductor for various electronic and optoelectronic applications. This work suggests that the component‐fusion‐based topology designer is a novel approach to tailor 2D materials with expected structures and interesting properties.