Nonvolatile memory is an indispensable component of electronic devices. However, the current technology makes it difficult to satisfy the emerging big data demand. To circumvent the existing problems, herein, a first attempt is made to achieve multifunctional nonvolatile memory based on all 2D heterostructures, consisting of histidine‐doped molybdenum disulfide quantum disks mixed with graphene oxide and a graphene macroscopic heterojunction. The designed device possesses intriguing hybrid electrically and optically controllable nonvolatile memory functionalities. By harnessing the unique properties of these materials, memory devices demonstrate long‐term stability and nonvolatile characteristics under both optical and electrical control signals. These devices possess outstanding features, such as multiple read‐write cycles, multi levels, and fast switching speeds, overcoming the limitations of traditional components. To explore the underlying physical mechanism, the Fermi level of graphene is measured and it is confirmed that the charge transfer and trapping across the heterojunctions are the major factors responsible for the observed behavior. This study demonstrates that 2D heterostructures for hybrid optically and electrically controllable nonvolatile memory pave an alternative route for the next‐generation information technology. 2D heterostructures for hybrid optically and electrically controllable nonvolatile memory are demonstrated that have excellent capability for applications in the next‐generation information technology.