“…Compared with synthetic organic hole-transport materials (HTM), cuprous thiocyanate (CuSCN) is regarded as a cheap but effective inorganic HTM for the fabrication of perovskite solar cells (PSCs), owing to abundant copper reserves on the earth, − high charge mobility, excellent energy level alignment, and satisfactory chemical stability. − So far, CuSCN-based PSCs have attained a certified champion power conversion efficiency (PCE) of 20.4% . Furthermore, compared to organic HTMs, CuSCN is found to protect perovskite layers from oxygen and moisture attack. − All of these advantages promise a bright prospect for CuSCN-based perovskite solar cells. − However, CuSCN has limited application in solution-processed PSCs due to its poor solubility. − The solvents for dissolving CuSCN are only a few short-chain n -alkyl sulfides and diethyl sulfides (DES), but they are likely to destroy perovskite layers simultaneously. − This results in an Ohmic contact degradation between the perovskite and CuSCN layers, which further weakens the power conversion efficiency of PSCs. − …”