AbstractIn this work, the drying step for cathodes based on carbon‐coated LiFePO4 prepared in the temperature range of 60–120 °C has been investigated in detail. The microstructure of the cathode shows a homogeneous distribution of the active material and conductive additive particles independent of the drying temperature. However, the results of impedance spectroscopy and cycling voltammetry are affected by the drying temperature. The solvent evaporation temperature, therefore, affects the polymer binder distribution and its characteristics, which include the polar phase content of the polymer and its affinity with the other components of the cathode. The discharge capacity value after 50 cycles is 120 and 81 mAh g−1 for the samples dried at 80 and 60 °C, respectively, which show the best and worst battery performance, respectively. It was concluded that carbon‐coated LiFePO4 cathodes should be prepared at drying temperatures between 80 and 100 °C for optimized performance.