fabrication of perovskite materials provide the feasibility of preparing flexible PSCs (F-PSCs), where their light-weight and bending-flexible properties, make this technology desirable in various occasions such as wearable bioelectronics, portable power equipment, deployable tents, etc. [7] Nowadays, with continuous developments in device structure and materials processing, PCEs of F-PSCs in laboratory have exceeded 21% in small-area (<0.1 cm 2 ) [8,9] and 15% in large-area (100 cm 2 ) [10] solar cell devices, thus showing promises in future flexible PV applications.F-PSCs are fabricated via replacing conventional rigid glass substrates with flexible substrates (e.g., polyethylene terephthalate (PET), and polyethylene naphthalate (PEN)). However, owing to the heat and chemically vulnerable nature of most organic materials, flexible substrate cannot withstand excessively high temperature without losing its elastic properties and therefore presents multiscale challenges that would hinder device performance. First of all, halide perovskites generally have inferior mechanical adhesion with adjacent functional layers or substrates due to their low cohesion energies, [11,12] while the large thermal expansion/contraction of flexible substrates during heat treatment will exacerbate such interfacial adhesion, thus rendering charge transport and mechanical durability in F-PSCs outstanding issues. [13] To achieve low-temperature processable functional layers, SnO 2 has been most frequently used as electron transport layer (ETL) in F-PSCs. [14] However, it presents unsatisfying interfacial electronic compatibility such as surface defects, lattice mismatch and large conduction band offset (ΔE CB ) with perovskite layer. [15,16] In addition, due to the discrepant physical properties (e.g., thermal expansivity) between organiccontaining perovskite and inorganic SnO 2 , perovskite/SnO 2 interface also contributes to phenomenal interfacial residual stress [17,18] and thus the consequent mechanical delamination, [13] once again affecting the PV performance and long-term durability of F-PSCs. To tackle the perovskite/SnO 2 interface problem, previous work included formamidinium iodide (FAI) in SnO 2 layer that consequently formed porous and interpenetrating interface between SnO 2 and perovskite for robust mechanical durability in F-PSCs. [19] While precise control of SnO 2 surface morphology and thickness enabled high-quality perovskite film formation with reduced trap-state density and Halide perovskites have shown superior potentials in flexible photovoltaics due to their soft and high power-to-weight nature. However, interfacial residual stress and lattice mismatch due to the large deformation of flexible substrates have greatly limited the performance of flexible perovskite solar cells (F-PSCs). Here, ammonium formate (HCOONH 4 ) is used as a preburied additive in electron transport layer (ETL) to realize a bottom-up infiltration process for an in situ, integral modification of ETL, perovskite layer, and their interface. The ...