In viewing underlying pathology with medical imaging, often specific material components contain most of the diagnostic information. Therefore, material component separation is desirable in many medical applications. Recent generations of MRI and X-ray CT systems can collect multiple measured data sets by changing data acquisition parameters, e.g., pulse sequence timing parameters in MRI and X-ray tube voltage in CT. These systems allow one to separate images of material components. In this thesis, we present novel image decomposition methods for MRI and X-ray CT applications. These methods use regularization and multiple data sets. We also propose iterative algorithms to minimize appropriate regularized least-squares cost functions. In MR ...