We propose to use a 3D MRF technique with multi-axis spiral projection acquisition to achieve 3D high-resolution whole-brain quantitative imaging for patients with MTLE. Isotropic 1-mm resolution relaxivity maps were achieved within 5 minutes. By incorporating Freesurfer’s automatic subcortical segmentation, a whole-brain subcortical segmentation was obtained, enabling feasible and subjective quantitative analysis for each substructure. Additionally, volume information of the substructure was obtained during the process.