efficiency (PCE) of rigid-substrate-based devices has exceeded 25%. [2] Meanwhile, flexible devices have also reached the highest PCE of 21.05%. [3] The merits of PSCs, such as low cost, suitable bandgaps for indoor light sources such as lightemitting diodes (LEDs), and simply fabricating flexible devices, [4][5][6][7] also enhance the indoor commercialization possibility. [8] In the past several years, research on indoor photovoltaics has also accelerated, which promotes the realization of the idea of the indoor Internet of Things (IoT) in the future. [9] The surfaces of indoor small electronic devices are usually irregularly curved. Compared to devices with rigid substrates, flexible devices can better fit the surface of small electrical appliances, which can increase the effective functional area and widen the application field range. [10] As the demand for adaptation to various indoor application scenarios, the mechanical stability of flexible devices is a very important concern. [11][12][13][14] Herein, we get inspiration from the balloon glue. The reason that balloon glue can deform so sharply but not break contributes to the cross-linking agent borax (Na 2 B 4 O 7 ). Borax is a common crosslinking agent that has excellent flexibility. The oxygen ion groups at both sides of the molecule can form stronger coordination bonds with lead than the lead-iodine bond, thereby acting as a stretch bridge at grain boundaries of perovskite films. We conducted physical tensile tests and extreme temperature variation tests (−180 to 150 °C) on the optimized films and found that the treated films exhibited better mechanical stability and phase stability. To prove the indoor application prospects of flexible devices, we first systematically reported the trap density of states of flexible devices under different light intensities. It is found that the trap density of formamidinium-lead-iodide (FAPbI 3 )-based perovskite is reduced after optimization, which is more suitable for indoor applications. [15,16] Meanwhile, since the improved film formation quality of perovskite contributed to passivation treatment of borax, the champion PCE of optimized rigid and flexible PSCs reached 23.05% and 21.63%, respectively, under AM 1.5G illumination. Moreover, the flexible device presents an a superior indoor PCE of 31.85% under 1062 lux (LED, 2956 K), which is currently the best flexible perovskite indoor photovoltaic device.Perovskite photovoltaics are strong potential candidates to drive low-power off-grid electronics for indoor applications. Compared with rigid devices, flexible perovskite devices can provide a more suitable surface for indoor small electronic devices, enabling them have a broader indoor application prospect. However, the mechanical stability of flexible perovskite photovoltaics is an urgent issue solved. Herein, a kind of 3D crosslinking agent named borax is selected to carry out grain boundary penetration treatment on perovskite film to realize full-dimensional stress release. This strategy improves the mechanical a...