In this paper, we propose a nonlinear structural hashing approach to learn compact binary codes for scalable video search. Unlike most existing video hashing methods which consider image frames within a video separately for binary code learning, we develop a multi-layer neural network to learn compact and discriminative binary codes by exploiting both the structural information between different frames within a video and the nonlinear relationship between video samples. To be specific, we learn these binary codes under two different constraints at the output of our network: 1) the distance between the learned binary codes for frames within the same scene is minimized and 2) the distance between the learned binary matrices for a video pair with the same label is less than a threshold and that for a video pair with different labels is larger than a threshold. To better measure the structural information of the scenes from videos, we employ a subspace clustering method to cluster frames into different scenes. Moreover, we design multiple hierarchical nonlinear transformations to preserve the nonlinear relationship between videos. Experimental results on three video data sets show that our method outperforms state-of-the-art hashing approaches on the scalable video search task.