Non-invasive measurements are important for the development of new treatments for heart failure, which is one of the leading causes of death worldwide. This study aimed to develop realistic subject-specific computational models of human biventricles using clinical data. Three-dimensional finite element models of the human ventricles were created using cardiovascular magnetic resonance images of rheumatic heart disease (RHD) patients and healthy subjects. The material parameter optimization uses inverse modeling based on the finite element method combined with the Levenberg–Marquardt method (LVM) by targeting subject-specific hemodynamics. The study of elastic myocardial parameters between healthy subjects and RHD patients showed an elevated stiffness in diseased hearts. In particular, the anisotropic material behavior of the healthy and diseased cardiac tissue significantly differed from one another. Furthermore, as the LVEF decreased, the stiffness and its orientation-dependent parameters increased. The simulation-derived LV myocardial circumferential and longitudinal stresses were negatively associated with the LVEF. The sensitivity analysis result demonstrated that the observed significant difference between the elastic material parameters of diseased and healthy myocardium was not exclusively attributable to an increased LVEDP in the diseased heart. These results could be applied to future computational studies for developing heart failure treatment.