<p>This study aimed to establish a noninvasive magnetic resonance angiography (MRA) framework for monitoring tumor vascular adaptation longitudinally using the intravascular supramolecular contrast agent 8-arm PEG-FGd₃. (1) Unlike conventional Gd-chelates, which predominantly enhanced tumor tissue because of contrast extravasation, 8-arm PEG-FGd₃ provided high-contrast delineation of tumor-feeding vessels and microvascular architecture, visualizing tumor vessels as small as 190&#xa0;μm. (2) This is the first instance of defining neovascularization patterns in superfine MRA images. (3) The longitudinal atlas of tumor vessels varied over time. In the fast-growing stage, both tumor doubling time and vessel doubling time were positive, vessels initiated neovascularization processes such as vessel co-option-like appearance, sprouting-like appearance, and elongation-tortuosity-like change. In the slow-growing stage, vessel doubling time turned negative, vessels became more structured, with continued elongation-tortuosity. Vessel remodeling followed vascular disruption rapidly. In the shrinkage stage, vessel loss preceded tumor shrinkage. (4) Seven days post-ligation, there were more vessels than the second day. ANG2 also showed a increasing tendency during this period, while VEGF was decreasing but still higher than that in the tumor without ligation, although there was no significant difference.</p>