Data security is a major concern in digital age, which generally relies on algorithm‐based mathematical encryption. Recently, encryption techniques based on physical principles are emerging and being developed, leading to the new generation of encryption moving from mathematics to the intersection of mathematics and physics. Here, device‐level encryption with ideal security is ingeniously achieved using modulation of the electron‐hole radiative recombination in a GaN‐LED. When a nano‐LED is driven in the non‐carrier injection mode, the oscillation of confined electrons can split what should be a single light pulse into multiple pulses. The morphology (amplitude, shape and pulse number) of those history‐dependent multiple pulses that act as carriers for transmitted digital information depends highly on the parameters of the driving signals, which makes those signals mathematically uncrackable and can increase the volume and security of transmitted information. Moreover, a hardware and software platform are designed to demonstrate the encrypted data transmission based on the device‐level encryption method, enabling recognition of the entire ASCII code table. The device‐level encryption based on splitting electroluminescence provides an encryption method during the conversion process of digital signals to optical signals and can improve the security of LED‐based communication.This article is protected by copyright. All rights reserved