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Low‐dimensional (LD) perovskite has provided an exciting avenue for exploring stable perovskite solar cells (PSCs). However, PSCs based on LD perovskites still suffer from poor efficiency owing to unfavorable charge carrier dynamics. Here, cystamine (CYS) is employed as a ligand to construct LD Dion‐Jacobson (LDDJ) perovskite (CYS)MAn‐1PbnI3n+1 (n = 1, 2, 3..., MA: methylamine) for improving carrier properties. The disulfide bond not only changes the polarization characteristic but also increases the coupling between inorganic slabs due to the low barrier of rotation around the S‐S axis, thus reducing the exciton binding energy of CYS‐based LDDJ perovskite. Disulfide bonds provide a scene for charge localization in the interlayer region, which is conducive to reducing the anisotropy of charge transfer. Thanks to these merits, the (CYS)MA4Pb5I16 film delivers improved carrier diffusion length (electron for 1345 nm and hole for 950 nm) and mobility (9.23 cm2 V−1 S−1). As a result, the (CYS)(MA)4Pb5I16 PSC achieves a champion power conversion efficiency (PCE) of 16.52%, which is much higher than that of HDA and BA cations‐based PSCs (HDA: 1,6‐Hexanediamine, BA: Butylamine). Furthermore, the state‐of‐the‐art device only lost 8% of its initial PCE after 1600 h in the atmosphere. [ABSTRACT FROM AUTHOR]

Low‐dimensional Ruddlesden‐Popper (LDRP) perovskites still suffer from inferior carrier transport properties. Here, we demonstrate that efficient exciton dissociation and charge transfer can be achieved in LDRP perovskite by introducing γ‐aminobutyric acid (GABA) as a spacer. The hydrogen bonding links adjacent spacing sheets in (GABA)2MA3Pb4I13 (MA=CH3NH3+), leading to the charges localized in the van der Waals gap, thereby constructing "charged‐bridge" for charge transfer through the spacing region. Additionally, the polarized GABA weakens dielectric confinement, decreasing the (GABA)2MA3Pb4I13 exciton binding energy as low as ≈73 meV. Benefiting from these merits, the resultant GABA‐based solar cell yields a champion power conversion efficiency (PCE) of 18.73 % with enhanced carrier transport properties. Furthermore, the unencapsulated device maintains 92.8 % of its initial PCE under continuous illumination after 1000 h and only lost 3 % of its initial PCE under 65 °C for 500 h. [ABSTRACT FROM AUTHOR]