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A large amount of low‐grade heat (<100 °C) is produced in electrical devices and mostly wasted. This type of heat without effective dissipation also causes compromised device performance, reliability, and lifespan. To tackle these issues, a redox targeting (RT)‐based flow cell with judiciously designed thermoelectrically active redox materials is demonstrated for the first time for efficient heat‐to‐electricity conversion through a thermally regenerative electrochemical cycle (TREC). Compared with the conventional TREC systems, the RT‐based flow cell not only reveals considerably enhanced thermoelectric efficiency, but the flow of redox fluids also provides a cooling function to the system. In this work, solid material Ni_0.2Co_0.8(OH)₂ and redox mediator [Fe(CN)₆]^4−/3−, both of which have negative temperature coefficient and share identical redox potential, are paired via RT‐reactions to boost the capacity and …