This paper proposes an effective method for accurately recovering vessel structures and intensity information from the X-ray coronary angiography (XCA) images of moving organs or tissues. Specifically, a global logarithm transformation of XCA images is implemented to fit the X-ray attenuation sum model of vessel/background layers into a low-rank, sparse decomposition model for vessel/background separation. The contrast-filled vessel structures are extracted by distinguishing the vessels from the low-rank backgrounds by using a robust principal component analysis and by constructing a vessel mask via Radon-like feature filtering plus spatially adaptive thresholding. Subsequently, the low-rankness and inter-frame spatio-temporal connectivity in the complex and noisy backgrounds are used to recover the vessel-masked background regions using tensor completion of all other background regions, while the twist tensor nuclear norm is minimized to complete the background layers. Finally, the method is able to accurately extract vessels’ intensities from the noisy XCA data by subtracting the completed background layers from the overall XCA images. We evaluated the vessel visibility of resulting images on real X-ray angiography data and evaluated the accuracy of vessel intensity recovery on synthetic data. Experiment results show the superiority of the proposed method over the state-of-the-art methods.