Piezoelectric energy harvesters (PEHs) aim to generate sufficient power to operate targeting device from the limited ambient energy. PEH includes mechanical-to-mechanical, mechanical-to-electrical, and electrical-to-electrical energy conversions, which are related to PEH structures, materials, and circuits, respectively; these should be efficient for increasing the total power. This critical review focuses on PEH structures and materials associated with the two major energy conversions to improve PEH performance. First, the resonance tuning mechanisms for PEH structures maintaining continuous resonance, regardless of a change in the vibration frequency, are presented. Based on the manual tuning technique, the electrically-and mechanicallydriven self-resonance tuning (SRT) techniques are introduced in detail. The representative SRT harvesters are summarized in terms of tunability, power consumption, and net power. Second, the figure-of-merits of the piezoelectric materials for output power are summarized based on the operating conditions, and optimal piezoelectric materials are suggested. Piezoelectric materials with large k ij , d ij , and g ij values are suitable for most PEHs, whereas those with large k ij and Q m values should be used for on-resonance conditions, wherein the mechanical energy is directly supplied to the piezoelectric material. This comprehensive review provides insights for designing efficient structures and selection of proper piezoelectric materials for PEHs.