The perovskite direct current nanogenerator (PDCG) is a novel energy conversion device with remarkable performance and comprehensive prospects. However, the interface of the perovskite Schottky junction still requires further optimization. Herein, an innovative approach by engineering a two-dimensional/three-dimensional (2D/3D) layered structure through phenylethylammonium iodide (PEAI) modification was introduced This novel modification significantly enhances the triboelectric effects in the Cs0.05(FA0.85MA0.15)0.95Pb(I0.85Br0.15)3/aluminum (CsFAMA/Al) Schottky junction PDCG, featuring a rolling structure. The PEAI-modified PDCG demonstrates a substantial improvement in performance, achieving an open circuit voltage (Voc) of 0.69 V, and a short circuit current (Isc) of 1.51 mA. Under 3 W illumination, the current density (Jsc) of PDCG with PEAI could achieve 92.81 A/m2, representing a 1.98-fold enhancement, realizing synergistic energy harvesting from mechanical and light energy. Furthermore, the innovative 2D/3D layer design significantly boosts the PDCG’s operational stability, reducing performance degradation. Notably, after a 9 h aging at 100°C, the Isc of the PDCG modified with PEAI maintained 85 % of its original value, a substantial improvement compared to the 68 % retention observed in the unmodified PDCG. The development of PDCG converting mechanical energy directly into direct current (DC) while possessing characteristics of integration and miniaturization, holds significant practical significance.