This paper proposes a deep hashing framework, namely Unsupervised Deep Video Hashing (UDVH), for largescale video similarity search with the aim to learn compact yet effective binary codes. Our UDVH produces the hash codes in a self-taught manner by jointly integrating discriminative video representation with optimal code learning, where an efficient alternating approach is adopted to optimize the objective function. The key differences from most existing video hashing methods lie in 1) UDVH is an unsupervised hashing method that generates hash codes by cooperatively utilizing feature clustering and a specifically-designed binarization with the original neighborhood structure preserved in the binary space; 2) a specific rotation is developed and applied onto video features such that the variance of each dimension can be balanced, thus facilitating the subsequent quantization step. Extensive experiments performed on three popular video datasets show that UDVH is overwhelmingly better than the state-of-the-arts in terms of various evaluation metrics, which makes it practical in real-world applications.