Models from the Vision Transformer (ViT) family have recently provided breakthrough results across image classification tasks such as ImageNet. Yet, they still face barriers to deployment, notably the fact that their accuracy can be severely impacted by compression techniques such as pruning. In this paper, we take a step towards addressing this issue by introducing Optimal ViT Surgeon (oViT), a new state-of-the-art method for the weight sparsification of Vision Transformers (ViT) models. At the technical level, oViT introduces a new weight pruning algorithm which leverages second-order information, specifically adapted to be both highly-accurate and efficient in the context of ViTs. We complement this accurate one-shot pruner with an in-depth investigation of gradual pruning, augmentation, and recovery schedules for ViTs, which we show to be critical for successful ViT compression. We validate our method via extensive experiments on classical ViT and DeiT models, as well as on newer variants, such as XCiT, EfficientFormer and Swin. Moreover, our results are even relevant to recently-proposed highly-accurate ResNets. Our results show for the first time that ViT-family models can in fact be pruned to high sparsity levels (e.g. ≥ 75%) with low impact on accuracy (≤ 1% relative drop), and that our approach outperforms prior methods by significant margins at high sparsities. In addition, we show that our method is compatible with structured pruning methods and quantization, and that it can lead to significant speedups on a sparsity-aware inference engine.