Metal-halide perovskites have attracted much attention for their excellent optoelectronic properties, such as tunable bandgap, long carrier lifetime, low cost, and lowtemperature solution-processibility. In just a few years, the power conversion efficiency (PCE) of perovskite solar cells (PSCs) has rapidly increased from 3.8% to more than 25%, [1,2] making them one of the most promising candidates for the nextgeneration low-cost photovoltaic technologies. This rapid progress is largely due to the careful modification of perovskite compositions, delicate design of device configurations, and an in-depth understanding of interfacial interactions, etc. [3][4][5][6] Inverted PSCs (p-i-n structure) have attracted increasing interest from both research and industry in recent years due to their little hysteresis and fatigue phenomena, low materials cost, simple preparation process, and readily scalable for largearea modules fabrication. [7][8][9][10][11] For p-i-n PSCs, the selection of hole transport layers (HTLs) is one of the most crucial steps for obtaining excellent device performance. p-type semiconductors, such as poly(3,4-ethylenedioxythiophene):poly-(styrenesulfonate) (PEDOT:PSS), polytriarylamine (PTAA), or nickel oxide (NiO X ) are commonly used HTLs to extract and transfer holes from the perovskite to the contact electrode. However, PEDOT: PSS has disadvantages in sensitivity to moisture because of its acidity, which potentially leads to the degradation of perovskites. [12] The poor wettability of PTAA makes the perovskite difficult to form dense films, which makes the devices prone to short circuits. [13] In contrast, NiO X is advantageous as an HTL due to its large bandgap (3.5-3.9 eV), deep valence band maximum (5.1-5.4 eV), high mobility (%10 À3 cm 2 V À1 s À1 ), [14][15][16] and intrinsic superior stability of the inorganic nature. In addition, NiO X HTL can be fabricated by a variety of scalable processing routes including chemical vapor deposition, [17] sputtering, [18,19] spray pyrolysis, [20][21][22] electron beam evaporation, [23] and so on. Among them, spray pyrolysis is a method that can fabricate large-area thin films at low cost, which is promising for scaling up PSCs. However, the solar cell performance based on spraycoated NiO X is inferior to the state-of-the-art PSCs, which urges the researchers to find a proper way to improve their performance.