Abstract The fast development of artificial intelligence has called for high-efficiency neuromorphic computing hardware. While two-dimensional floating-gate memories show promise, their limited state numbers and stability hinder practical use. Here, we report gate-injection-mode two-dimensional floating-gate memories as a candidate for large-scale neural network accelerators. Through a coplanar device structure design and a bi-pulse state programming strategy, 8-bit states with intervals larger than three times of the standard deviations and stability over 10,000 s are achieved at 3 V. The cycling endurance is over 105 and the fabricated 256 devices show a yield of 94.9%. Leveraging this, we carry out experimental image convolutions and 38,592 kernels transplanting on an integrated 9 × 2 array that exhibits results matching well with simulations. We also show that fix-point neural networks with 8-bit precision have inference accuracies approaching the ideal values. Our work validates the potential of gate-injection-mode two-dimensional floating-gate memories for high-efficiency neuromorphic computing hardware.