Quantitative myelin content imaging provides novel and pertinent information related to underlying pathogenetic mechanisms of myelin-related disease or disorders arising from aberrant connectivity. Multicomponent driven equilibrium single pulse observation of T1 and T2 is a time-efficient multicomponent relaxation analysis technique that provides estimates of the myelin water fraction, a surrogate measure of myelin volume. Unfortunately, multicomponent driven equilibrium single pulse observation of T1 and T2 relies on a two water-pool model (myelin-associated water and intra/extracellular water), which is inadequate within partial volume voxels, i.e., containing brain tissue and ventricle or meninges, resulting in myelin water fraction underestimation. To address this, a third, nonexchanging “free-water” component was introduced to the multicomponent driven equilibrium single pulse observation of T1 and T2 model. Numerical simulations and experimental in vivo data show that the model to perform advantageously within partial volume regions while providing robust and reproducible results. It is concluded that this model is preferable for future studies and analysis. Magn Reson Med, 2013. © 2012 Wiley Periodicals, Inc.