The low output current density of piezoelectric nanogenerators (PENGs) severely restricts their application for ambient mechanical energy harvest. This has been a key challenge in the development of PENG. Here, to conquer this, based on a piezoelectric material with high piezoelectric coefficient (Sm-PMN-PT), a new design of PENG with a three-dimensional intercalation electrode (IENG) is proposed. By creating many boundary interfaces inside the piezoelectric material, the total amount of surface polarization charges increased, which contributes to an increased current density. The IENG can output a maximum peak shortcircuit current of 320 μA, and the corresponding current density 290 μA cm −2 is 1.93 and 1.61 times the record values of PENG and triboelectric nanogenerator (TENG), respectively. It can also charge a 1 μF capacitor from 0 V to 8 V in 21 cycles, and the equivalent surface charge density 1690 μC m −2 is 1.35 times the record value of TENG.