It has been previously shown that high-quality partial volume tissue compartment maps can be obtained by combining multiparametric contrast-encoded MRI data acquisition methods with spatially-regularized spectroscopic image estimation techniques. However, the advantages of this combined approach generally come at the expense of substantial computational complexity. In this work, we propose a new algorithm to solve this kind of estimation problem more efficiently. Our algorithm is based on the linearized alternating directions method of multipliers (LADMM), and relies on the introduction of novel quadratic penalty terms to substantially simplify the subproblems that must be solved at each iteration. We evaluate this algorithm on a variety of different estimation problems (diffusion-relaxation, relaxation-relaxation, relaxometry, and magnetic resonance fingerprinting), where we consistently observe substantial (roughly 5$\times$-80$\times$) speed improvements. We expect that this new faster algorithm will lower practical barriers to using spatial regularization and multiparametric contrast-encoded MRI data acquisition methods for partial volume compartment mapping.