 This study presents a new hypersensitive Mr. Angiography strategy using zwaterionic GD-Kelate contrast agents, PAAGD, that have improved longitudinal molar relaxivity, blood half-life, and low immunogenicity compared to individual GD cellets. The PAAGD strategy enables sophisticated microvessals angiography with a resolution at the order of 100 micrometers, and has been evaluated on animal models of cardiac cerebrovascular diseases using a 7.0 TMI scanner and clinical translation potential on swine using a 3.0 T clinical MI scanner. The current study offers a promising strategy for precise diagnosis of vascular diseases. This article was authored by Paixin Zhong, Junwei Cheng, Yijie Lu, and others.