Abstract: In multivariate regression models, a sparse singular value decomposition of the regression component matrix is appealing for reducing dimensionality and facilitating interpretation. However, the recovery of such a decomposition remains very challenging, largely due to the simultaneous presence of orthogonality constraints and co-sparsity regularization. By delving into the underlying statistical data-generation mechanism, we reformulate the problem as a supervised co-sparse factor analysis, and develop an efficient computational procedure, named sequential factor extraction via co-sparse unit-rank estimation (SeCURE), that completely bypasses the orthogonality requirements. At each step, the problem reduces to a sparse multivariate regression with a unit-rank constraint. Nicely, each sequentially extracted sparse and unit-rank coefficient matrix automatically leads to co-sparsity in its pair of singular vectors. Each latent factor is thus a sparse linear combination of the predictors and may influence only a subset of responses. The proposed algorithm is guaranteed to converge, and it ensures efficient computation even with incomplete data and/or when enforcing exact orthogonality is desired. Our estimators enjoy the oracle properties asymptotically; a non-asymptotic error bound further reveals some interesting finite-sample behaviors of the estimators. The efficacy of SeCURE is demonstrated by simulation studies and two applications in genetics. Supplementary materials for this article are available online.