Cardiac magnetic resonance is the gold standard for evaluating left-ventricular ejection fraction (LVEF). Standard protocols, however, can be inefficient, facing challenges due to significant operator and patient involvement. Although the free-running framework (FRF) addresses these challenges, the potential of the extensive data it collects remains underutilized. Therefore, we propose to leverage the large amount of data collected by incorporating interbin cardiac motion compensation into FRF (FRF-MC) to improve both image quality and LVEF measurement accuracy, while reducing the sensitivity to user-defined regularization parameters. FRF-MC consists of several steps: data acquisition, self-gating signal extraction, deformation field estimations, and motion-resolved reconstruction with interbin cardiac motion compensation. FRF-MC was compared with the original 5D-FRF method using LVEF and several image-quality metrics. The cardiac regularization weight ( ) was optimized for both methods by maximizing image quality without compromising LVEF measurement accuracy. Evaluations were performed in numerical simulations and in 9 healthy participants. In vivo images were assessed by blinded expert reviewers and compared with reference standard 2D-cine images. Both in silico and in vivo results revealed that FRF-MC outperformed FRF in terms of image quality and LVEF accuracy. FRF-MC reduced temporal blurring, preserving detailed anatomy even at higher cardiac regularization weights, and led to more accurate LVEF measurements. Optimized produced accurate LVEF for both methods compared with the 2D-cine reference (FRF-MC: 0.59% [-7.2%, 6.0%], p = 0.47; FRF: 0.86% [-8.5%, 6.7%], p = 0.36), but FRF-MC resulted in superior image quality (FRF-MC: 2.89 ± 0.58, FRF: 2.11 ± 0.47; p < 10-3). Incorporating interbin cardiac motion compensation significantly improved image quality, supported higher cardiac regularization weights without compromising LVEF measurement accuracy, and reduced sensitivity to user-defined regularization parameters.