[1] Sparse geologic dictionaries provide a novel approach for subsurface flow model representation and calibration. Learning sparse dictionaries from prior training data sets is an effective approach to describe complex geologic connectivity patterns in subsurface imaging applications. However, the computational cost of sparse learning algorithms becomes prohibitive for large models. Performing the sparse dictionary learning process on smaller image patches (segments) provides a simple approach to address this problem in image processing applications. However, in underdetermined subsurface flow model calibration inverse problems, reconstruction of a segmented image can introduce significant structural distortion and discontinuity at the boundaries of the segments. This paper proposes an alternative sparse learning approach where the sparse dictionaries are learned from low-rank representations of the large-scale training data set in spectral domains (e.g., frequency domain). The objective is to develop a computationally efficient dictionary learning approach that emphasizes large-scale spatial connectivity patterns. This is achieved by removing the strong spatial correlations in the training data, thereby eliminating a large number of insignificant components from the sparse learning computation. In addition to improving the computational complexity, sparse learning from low-rank training data sets suppresses the small-scale details from entering the reconstruction of large-scale connectivity patterns, thereby providing a regularization effect in solving the resulting ill-posed inverse problems. We apply the proposed approach to travel-time tomography inversion and nonlinear subsurface flow model calibration inverse problems to demonstrate its effectiveness and practicality.