Heart failure is a chronic disease that causes repeat hospitalizations, reduced quality of life and increased mortality, and is a major global healthcare burden. Cardiac imaging facilitates heart failure diagnosis, elucidation of the etiology, monitoring of progression and prognostication. Comprehensive assessment of myocardial tissue characteristics as well as systolic and diastolic functional parameters in the ventricles and atria are needed to diagnose heart failure, especially in heart failure with preserved ejection. Cardiac magnetic resonance (CMR) is an imaging modality that yields high-quality images of all heart chambers, and is the reference standard for measurement of left ventricular ejection fraction. However, conventional CMR analyses fail to exploit the rich 4D spatiotemporal information contained in the CMR image dataset, which we believe can be unlocked using the appropriate methods for comprehensive quantitation of left and right ventricular, as well as atrial systolic and diastolic functions. We pioneered computational post-processing techniques that can quantitate regional ventricular function as well as measure phasic atrial strains and their corresponding strain rates. The proof-of-concept and validation of these novel parameters, as well as relevant clinical applications, will be discussed.