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Neuromorphic computing, which mimics the structure and principles of the human brain, has the potential to facilitate the hardware implementation of next-generation artificial intelligence systems and process large amounts of data with very low power consumption. Among them, the XNOR synapse-based Binary Neural Network (BNN) has been attracting attention due to its compact neural network parameter size and low hardware cost. The previous XNOR synapse has drawbacks, such as a trade-off between cell density and accuracy. In this work, we show nonvolatile XNOR synapses with high density and accuracy using a monolithically stacked complementary ferroelectric field-effect transistor (C-FeFET) composed of a p-type Si MFMIS-FeFET at the bottom and a 3D stackable n-type Al:IZTO MFS-FeTFT, achieving 60F 2 per cell (2C-FeFET). For adjusting the threshold voltage and improving the switching speed (100 ns) of n-type ferroelectric TFT, we employed a dual-gate configuration and a unique operation scheme, making it comparable to those of Si-based FeFETs. We performed array-level simulation with a 512 × 512 subarray size and a 3-bit flash ADC, demonstrating that the image recognition accuracies using the MNIST and CIFAR-10 data sets were increased by 3.17 and 14.07%, respectively, in comparison to other nonvolatile XNOR synapses. In addition, we performed system-level analysis on a 512 × 512 XNOR C-FeFET, exhibiting an outstanding throughput of 717.37 GOPS and an energy efficiency of 196.7 TOPS/W. We expect that our approach would contribute to the high-density memory systems, logic-in-memory technology, and hardware implementation of neural networks.