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Lead-free piezoelectric one-dimensional (1D) nanostructures have exhibited great potential in building biocompatible micro/nano-energy harvesters and self-powered smart sensors. However, their low piezoelectric coefficient still remains as the biggest obstacle for practical applications. In this work, an ultrahigh piezoelectric coefficient with calibrated d33from 400 pm V-1to 814 pm V-1is achieved in Li-doped (K,Na)NbO3(KNLN) lead-free piezoelectric nanorod arrays (NRAs). The giant enhancement on the piezoelectric performance of the KNLN nanorods can be attributed to the manipulation on the phase transition behavior together with the relaxation of strain. The Li+dopants induce large NbO6octahedral distortion and result in the decreased phase transition temperature from orthorhombic (O) to tetragonal (T) phase, which leads to the construction of the O-T phase boundary at room temperature and improves the polarization performance of the products. The ultrahigh piezoelectric performance of the KNLN NRAs gives rise to the remarkably improved energy harvesting performance, which shows highly sensitive pressure sensing behaviors and can be utilized for monitoring the human-body motions.