AbstractPiezoelectric energy harvesting technology is drawing substantial attention as an eco‐friendly method to promote energy transformation, which is at the forefront of current scientific research. However, the difficulties involved in obtaining a stable output voltage (Vout) and a controllable output current density (Iout) represent bottlenecks in the development of piezoelectric energy harvesters (PEHs) for practical applications. Here, a novel strategy that couples elastic polarization configuration with activity rattling space in lead‐free potassium sodium niobate‐based piezoceramics is proposed to break through this barrier. The cantilever beam‐type PEHs assembled using the rationally designed piezoceramic system show a stable Vout (≈22 V) and a controllable Iout over the range from 6.09 to 20.16 µA cm−2, which is sufficient to drive multiple types of wireless sensors that have the same rated voltage but different rated current requirements. These fantastic power generation performances are associated with a stable piezoelectric voltage coefficient (g33), an increasing piezoelectric charge coefficient (d33), and a weakened electrostrictive coefficient (Q33) that stem from polarization configuration optimization in combination with introduction of the activity rattling space design. This work provides a good approach to modulation of the overall performance of piezoelectric materials to meet the demands of advanced PEH applications.
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