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Model binarization can significantly compress model size, reduce energy consumption, and accelerate inference through efficient bit-wise operations. Although binarizing convolutional neural networks have been extensively studied, there is little work on exploring binarization of vision Transformers which underpin most recent breakthroughs in visual recognition. To this end, we propose to solve two fundamental challenges to push the horizon of Binary Vision Transformers (BiViT). First, the traditional binary method does not take the long-tailed distribution of softmax attention into consideration, bringing large binarization errors in the attention module. To solve this, we propose Softmax-aware Binarization, which dynamically adapts to the data distribution and reduces the error caused by binarization. Second, to better preserve the information of the pretrained model and restore accuracy, we propose a Cross-layer Binarization scheme that decouples the binarization of self-attention and multi-layer perceptrons (MLPs), and Parameterized Weight Scales which introduce learnable scaling factors for weight binarization. Overall, our method performs favorably against state-of-the-arts by 19.8% on the TinyImageNet dataset. On ImageNet, our BiViT achieves a competitive 75.6% Top-1 accuracy over Swin-S model. Additionally, on COCO object detection, our method achieves an mAP of 40.8 with a Swin-T backbone over Cascade Mask R-CNN framework.