MRI techniques that utilize the magnetization transfer (MT) effect are highly desirable as they potentially can map the myelin content. However, MT measurements produced by conventional MT-MRI techniques, such as MT ratio imaging, vary with the pulse sequence and the scan parameters used. The MT effect and the intrinsic spin–lattice relaxation, both a component of the MR longitudinal relaxation, must be separated to improve MT-MRI accuracy and precision. To solve the problem, a method for MT-MRI is developed in this work. In patients of multiple sclerosis, the present MT-MRI shows improved specificity to demyelinating lesions in the brain.