The integration of logic, memory, and neuromorphic functions within a single electronic platform is a central goal for next‐generation information technologies. Two‐dimensional (2D) materials, with their atomic thickness and tunable electronic properties, offer an ideal foundation for multifunctional device architectures. However, realizing complementary operation in 2D electronics remains challenging due to the scarcity of stable p‐type semiconductors and the difficulty of controlling interfacial charge transfer. Here, we demonstrate interface‐engineered complementary field‐effect transistors (cFETs) based on molybdenum diselenide (MoSe2) and MoSe2/chromium oxychloride (CrOCl), enabling tunable n‐ and p‐type conduction via van der Waals interfacial coupling. Pristine MoSe2 exhibits n‐type transport with an electron mobility of approximately 18 cm2 V−1 s−1, while charge transfer from CrOCl induces robust p‐type conduction with a hole mobility of about 1.1 cm2 V−1 s−1, allowing the realization of balanced resistive‐load and CMOS inverter circuits with noise margins up to 40% of the supply voltage. Compared with conventional 2D FETs, this approach achieves simultaneous logic, nonvolatile memory, and synaptic functionalities within a single device, demonstrating multilevel data storage and long‐term synaptic plasticity. These results reveal that interface coupling in MoSe2/CrOCl heterostructures enables precise polarity control without chemical doping, overcoming a key limitation of 2D electronics. Overall, this work establishes MoSe2/CrOCl cFETs as a versatile platform bridging digital logic, memory, and neuromorphic computing within all‐2D architectures.
Viscardi et al. (Sun,) studied this question.