Memristors integrated with low operating voltage, good stability, and environmental benignity play an important role in data storage and logical circuit technology, but their fabrication still faces challenges. This study reports an ultra-thin bio-memristor based on pristine environment-friendly silk nanofibrils (SNFs). The intrinsic ionic conductivity, combined with high dielectric performance and nanoscale thickness, lowers the operation voltage down to 0.1–0.2 V, and enables stable switching and retention time over 180 times and 105 s, respectively. Furthermore, the SNF-based memristor device in a crossbar array achieves stable memristive performance, and thus realizes the functions of memorizing image and logic operation. By carrying out variable-temperature electrical experiments and Kelvin probe force microscopy, the space charge-limited conduction mechanism is revealed. Integrating with low operating voltage, good stability, and ultra-thin thickness makes the SNF-based memristors excellent candidates in bioelectronics.