This research aims to develop the flexible triboelectric nanogenerator (TENG) using PDMS polymer as the main tribo-material and composite with dielectric rare earth oxide, lanthanum chromite compound; LaCrO3, to enhance generated charge density, before add-on its higher electrical output with gamma ray irradiation. Upon study the effect of different amounts of the loaded LaCrO3 and various doses of gamma ray, the optimum condition can be obtained. The PDMS/LaCrO3 at 5 wt% can reach open-circuit voltage (VOC) and shot-circuit current (ISC) at 89 V and 448 μA. The impressive results of output further appear by additional irradiated gamma radiation. At 150 kGy dose of Irradiated gamma ray, VOC and ISC can jump to 161 V and 963 μA. These output signals, especially ISC, can be ∼34 times higher than that of the pristine PDMS. Scientific discussion regarding characterization, operating mechanism, dielectric properties and electrical output is provided. The practical application of being a small power source is also developed. Therefore, this research can show another useful application of gamma ray in the field of materials design for energy harvesting devices. The knowledge provided in this research can also serve as potential guidance in the field of specific TENG utilization.