“…[ 7 ] Despite the sky‐rocketing progress in efficiency, the moisture and thermal instability of 3D PSCs hinder the future commercialization. [ 8–10 ] To improve stability, quasi 2D (Q‐2D) Ruddlesden–Popper (RP) perovskites have been adopted owing to their better moisture stability, stemming from hydrophobic bulky organic cations which resist moisture invasion into the perovskite lattice. [ 11,12 ] Typically, such Q‐2D RP perovskites are expressed as (R‐NH 3 ) 2 A n −1 M n X 3 n +1 ( n = 1, 2, 3, 4…), where R‐NH 3 is primary aromatic or aliphatic alkylammonium spacer cation (e.g., phenethylammonium (PEA + ), butylammonium (BA + )), A is an interstitial cation (e.g., Cs + , methylammonium (MA + ), formamidinium (FA + )), M is a divalent metal cation (e.g., Pb 2+ , Sn 2+ ), X is a halide anion (e.g., I − , Br − , Cl − ), and n is the layer number of inorganic [MX 6 ] 4− octahedral slabs between two R‐NH 3 spacers.…”