In this thesis, we study the problem of recovering signals, in particular images, that approximately satisfy severely ill-conditioned or underdetermined linear systems. For example, such a linear system may represent a set of under-sampled and noisy linear measurements. It is well-known that the quality of the recovery critically depends on the choice of an appropriate regularization model that incorporates prior information about the target solution. Two of the most successful regularization models are the Tikhonov and Total Variation (TV) models, each of which is used in a wide range of applications. We design and investigate a class of spectrum-based models that generalize and improve upon both the Tikhonov and the TV methods, as well as their combinations or so-called hybrids. The proposed models contain "spectrum parameters" that are learned from training data sets through solving optimization problems. This parameter-learning feature gives these models the flexibility to adapt to desired target solutions. We devise efficient algorithms for all the proposed models and conduct comprehensive numerical experiments to evaluate their performance as compared to established models. Numerical results show a generally superior quality in recovered images by our approach from under-sampled linear measurements. Using the proposed algorithms, one can often obtain much improved quality at a moderate increase in computational time.