One of the main challenges with implantable biomedical devices is the replacement surgeries of depleted batteries for elderly patients. This not only poses medical risks but also results in financial burdens. Consequently, there is a growing need for self-powered in vivo electronics that can convert the biomechanical movements of organs into usable electric energy. Notably, a previously reported in vivo flexible energy harvester generated relatively low current output from a living porcine heart, restricting its ability to operate self-powered electronic devices. In this study, a high current output implantable flexible energy harvester was demonstrated by adopting a highly-piezoelectric single crystal Pb(In1/2Nb1/2)O3–Pb(Mg1/3Nb2/3)O3–PbTiO3 (PIN–PMN–PT) film. The in vivo flexible energy harvester generated a short-circuit output current of 20 µA (corresponding to a current density of 3.08 µA/mm3) from the contraction and relaxation of a porcine heart. This recorded in vivo output current density was attributed to its outstanding piezoelectric charge coefficient of the single crystal PIN-PMN-PT, optimized Ni stressor assisted exfoliation as well as the implementation of a metal-insulator-metal (MIM) structure. Moreover, the flexible energy harvester was also demonstrated as a self-powered cardiac sensor to monitor irregular heartbeats by observing heart rate variations due to drug administration in a porcine heart. Additionally, output performance evaluation was conducted with the chest closed to further assess the feasibility of practical in vivo harvesting. Finally, the single crystal harvester exhibited biocompatibility, showing no signs of cytotoxicity based on cell viability assessments and histological characterizations. These results underscore the potential of the flexible PIN-PMN-PT energy harvesting device as a sustainable power source for self-powered in vivo biomedical electronics.