Introduction: Conventional CMR exams for assessment of cardiac anatomy and tissue characterization require multiple sequential 2D acquisitions under breath-hold in different orientations, in addition to being limited to 1.5 T and 3 T. Methods: In this study, we sought to develop a novel 3D motion-compensated free-breathing sequence for comprehensive high-resolution whole-heart assessment of cardiovascular anatomy via simultaneous bright- and black-blood imaging and co-registered (Formula presented.) myocardial tissue quantification in a one-click scan at 0.55 T. Results: Good agreement with a spin-echo reference sequence was found in the phantom for (Formula presented.) mapping. In-vivo, the proposed research sequence was evaluated in 10 healthy subjects, providing great delineation of cardiac and vascular structures, good visibility of coronary arteries and accurate (Formula presented.) parametric mapping in a clinically feasible time of less than 9 min.