Magnetic resonance angiography (MRA) is pivotal for diagnosing panvascular diseases. However, single-modality MRA falls short in diagnosing diverse vascular abnormalities. Thus, contrast agents combining and effects are sought for multiparameter MRA with clinical promise, yet achieving a balance in and contrast enhancement effects remains a scientific challenge. Herein, we developed a hypersensitive multiparameter MRA strategy using dual-modality NaGdF nanoparticles. Because of the longer tumbling time (τ), NaGdF nanoparticles can improve the longitudinal relaxivity (), brightening vessels in -weighted sequences. Simultaneously, the regular arrangement of Gd in the crystal induces magnetic anisotropy, creating local static magnetic field heterogeneity and generating negative signals in -weighted sequences. Consequently, the efficacy of NaGdF-enhanced high-resolution multiparameter MRA has been validated in diagnosing ischemic stroke and Alzheimer's disease in rodent models. In addition, the dual-contrast imaging has been realized on swine with a clinical 3.0-T magnetic resonance imaging scanner, highly emphasizing the clinical translation prospect.