Ultrafast Doppler has been accepted as a novel modality for small vasculature imaging with high sensitivity, high spatiotemporal resolution, and high penetration. However, the conventional Doppler estimator adopted in studies of ultrafast ultrasound imaging is only sensitive to the velocity component along the beam direction and has angle-dependent limitations. Vector Doppler has been developed with the goal of angle-independent velocity estimation but is typically employed for relatively large vessels. In this study, combining multiangle vector Doppler strategy and ultrafast sequencing, ultrafast ultrasound vector Doppler (ultrafast UVD) is developed for small vasculature hemodynamic imaging. The validity of the technique is demonstrated through experiments on a rotational phantom, rat brain, human brain, and human spinal cord. A rat brain experiment shows that compared with the ultrasound localization microscopy (ULM) velocimetry, which is widely accepted as an accurate flow velocimetry technique, the average relative error (ARE) of the velocity magnitude estimated by ultrafast UVD is approximately 16.2%, with a root-mean-square error (RMSE) of the velocity direction of 26.7°. It is demonstrated that ultrafast UVD is a promising tool for accurate blood flow velocity measurement, especially for the organs, including brain and spinal cord with vasculature typically exhibiting tendential alignment of vascular trees.