Hashing has been widely studied for cross-modal retrieval due to its promising efficiency and effectiveness in massive data analysis. However, most existing supervised hashing has the limitations of inefficiency for very large-scale search and intractable discrete constraint for hash codes learning. In this paper, we propose a new supervised hashing method, namely, Discrete Semantic Matrix Factorization Hashing (DSMFH), for cross-modal retrieval. First, we conduct the matrix factorization via directly utilizing the available label information to obtain a latent representation, so that both the inter-modality and intra-modality similarities are well preserved. Then, we simultaneously learn the discriminative hash codes and corresponding hash functions by deriving the matrix factorization into a discrete optimization. Finally, we adopt an alternatively iterative procedure to efficiently optimize the matrix factorization and discrete learning. Extensive experimental results on three widely used image-tag databases demonstrate the superiority of the DSMFH over state-of-the-art cross-modal hashing methods.