The explosive growth of massive‐data storage and the demand for ultrafast data processing require innovative memory devices with exceptional performance. Two‐dimensional (2D) materials and their van der Waal heterostructures with atomically sharp interfaces hold great promise for innovations in memory devices. Here, we present non‐volatile, floating‐gate memory devices with all functional layers made of 2D materials, achieving ultrafast programming/erasing speeds (20 ns), high extinction ratios (up to 108), and multi‐bit storage capability. These devices also exhibit long‐term data retention exceeding 10 years, facilitated by a high gate‐coupling ratio (GCR) and atomically sharp interfaces between functional layers. Additionally, we demonstrate the realization of an “OR” logic gate on a single‐device unit by synergistic electrical and optical operations. The present results provide a solid foundation for next‐generation ultrahigh‐speed, ultralong lifespan, non‐volatile memory devices, with a potential for scale‐up manufacturing and flexible electronics applications.This article is protected by copyright. All rights reserved