Solar photovoltaic (PV) energy is taking an increasingly important role all over the world. Among different solar cells, perovskite solar cells (PSCs) are regarded as the next-generation technology that could further decrease the manufacturing cost with comparable efficiency to silicon solar cells. Perovskite materials possess marvelous optoelectronic properties like high light absorption coefficient, tunable bandgap, and long charge diffusion length. [1][2][3][4][5][6][7][8] Recently, state-of-the-art devices have achieved tremendous progress with power conversion efficiencies (PCEs) exceeding 25%. [9][10][11] Besides, with the intrinsic mechanical flexibility and low-temperature processability, PSCs are able to be prepared on flexible substrates, which will broaden the application areas in portable electronics, wearable devices, and so on. [12][13][14][15][16][17] Moreover, PSCs could be fabricated by the roll-to-roll printing process, which has already been successfully demonstrated in the commercialization of organic PVs. Needless to say, flexible perovskite solar cells (FPSCs) have become a significant topic in practical applications of PSCs (See Figure 1). [18] Kumar et al. reported the first FPSC in 2013, and the PCE was only 2.62%. [19] In this work, polyethylene terephthalate (PET) was used as a flexible substrate, followed by low-temperature deposited ZnO nanorods. Currently, the record PCE of flexible devices is still lower than that of rigid ones. To some extent, the loss is inevitably caused by the trade-off between the requirement of mechanical flexibility for application and mechanical rigidity for fabrication. Different from rigid PSCs, the morphologies of the layers in FPSCs are difficult to control