Direct‐current triboelectric nanogenerators (DC‐TENGs) can directly convert mechanical energy into direct current (DC) electrical energy, exhibiting wide applications in micro/nano power sources, etc. Herein, a rolling‐mode DC‐TENG based on the tribo‐photovoltaic effect is proposed, which verifies that the tribovoltaic effect can be achieved in DC‐TENGs with a rolling structure instead of a conventional sliding structure. Utilizing the all‐inorganic perovskite CsPbBr3, a multifunctional DC‐TENG with excellent performance, that is capable of collecting both mechanical and solar energy is produced by constructing a dynamic Al/CsPbBr3 Schottky junction. Under illumination by light, the output voltage and current density reach 3.69 V and 11.46 A m−2, respectively. Furthermore, the output current of the dynamic Al/CsPbBr3 junction under illumination is 4.7 times higher than that in dark conditions. Meanwhile, the device exhibits excellent stability and the output performance does not significantly degrade after more than 10 min of cycling. In addition, the DC‐TENG shows potential applications in temperature and humidity sensing and directly charging capacitors. This work not only realizes a multifunctional DC‐TENG for simultaneously harvesting mechanical and solar energy, but also provides a novel route to enhance the work stability through a rolling‐mode device structure, which is of great significance for accelerating the development and applications of high‐performance DC‐TENGs.

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