Flexible and highly filled piezoelectric nanogenerators with excellent performance play an indispensable role in portable electronic devices, while the bottlenecks are hard to improve the polarization efficiency and prepare three-dimensional (3D) amplifying effect structure. Compared with other typical 3D printing technologies, direct ink writing multi-material printing (DIW-M3D), can extrude multiple viscoelastic ink materials with a wide selection of materials, which has the advantage of integrated multi-material processing. However, there are fewer reports on the use of DIW-M3D technology to print functional composite materials. Inspired from Lego block structures, we utilized DIW-M3D technology to prepare fabrications with alternating arrangements of piezoelectric and conductive inks between layers. This voxel-isolated conducting network provided the superior polarization path and uniform distribution of polarization field, which sharply ameliorate the piezoelectric effect and output performance. Owing to this voxel-isolated structure, the VOC and ISC could reach 150 V and 16 µA respectively, with the jumping movements of the forefoot. This work paved a path of scale-up preparing piezoelectric devices with 3D amplification effect structure and enhanced the polarization efficiency of the devices.