Developing multifunctional nanoelectronics will facilitate simplifying the circuits for future high‐integrated system. CuInP2S6 (CIPS) exhibiting ferroionic phenomena allows the manipulation of polarization and conductive behaviors. Here, a MoS2 transistor is fabricated with CIPS gate dielectric layer to realize the functions of nonvolatile memory, broadband photodetector and voltage comparator. It exhibited convex‐shaped anti‐ambipolar transfer characteristics, with a sharp boundary as the n‐/p‐type conductance conversion line, guiding the precise modulation of its working modes by tuning voltage. The CIPS works as a ferroelectric insulator to support the n‐type transistor, while as a semiconductor dominated by Cu+ migration to reconfigure a p‐type memristive transistor. It owns hysteresis behavior in both modes, demonstrating the n‐ and p‐type memory windows synchronously. Also, it exhibits the nonvolatile memory property with low energy‐consumption of 4 pJ per bite, good endurance of 2567 write‐erase cycles, and good retention with a high current on/off ratio of 2 × 103 over 104 s without any obvious decay. Moreover, it extends the photodetection from visible to near‐infrared with the responsivity of 321 AW−1 at 1200 nm wavelength. This work provides an effective strategy for the realization of multiple functions by specific materials and devices.