Cardiac Magnetic Resonance T1 mapping enables quantitative characterization of myocardium, which appeals huge attention from clinic. In this work, we proposed a free-breathing high-resolution three-dimensional (3D) T1 mapping sequence. By using variable flip Angle technique for readouts and saturation-recovery preparation for T1 weightings, the proposed sequence is highly efficient in acquisition of all volumes, including the one at the equilibrium of the longitudinal magnetization. Whole-heart pre- and post-contrast homogeneous T1 maps at an imaging resolution 1.25×1.25×8 mm3 were successfully obtained within 10 minutes in healthy volunteers. After rigid registration, 3D Extracellular Volume maps were eventually achieved.