Organic/inorganic hybrid perovskite solar cells (PeSCs) have been of great interest due to their easy fabrication and high power conversion efficiency (PCE) exceeding 25%. [1-4] Nevertheless, hybrid perovskites (PVKs) suffer from low thermal stability due to the volatile nature of organic cations (i.e., methylamine), [5] which limits the commercial applications of hybrid PeSCs. [6,7] Thus, inorganic cations such as Cs þ are used to replace organic cations, [8] yielding all-inorganic PVKs with considerably improved thermal stability. [9,10] Among various Cs-based inorganic PVKs, dual-halide PVKs of CsPbI 2 Br feature a suitable bandgap (E g) of around 1.9 eV and reasonable phase stability, [11] which make it a promising photoabsorber. To date, champion PCEs of 17.03% and 15.92% have been achieved for n-i-p-type (normal) and p-in (inverted)-type PeSCs, respectively, both based on CsPbI 2 Br. [12-18] Nevertheless, such PCE values are still lower than those of hybrid PeSCs. Further improvement is highly demanded for all-inorganic PeSCs. It has been well recognized that solution-processed inorganic PVK films, especially those prepared at a low temperature, are highly defective, [19] which usually result in large energy loss in PeSCs. For example, the highest reported open-circuit voltages (V OC) are 1.40 and 1.27 V for normal and inverted CsPbI 2 Br PeSCs, [15,16] respectively, both much lower than the E g (%1.9 eV) of PVK. Such large energy loss might be attributed to the severe defect-induced nonradiative recombination. [20,21] In addition, high-density interfacial defects also lead to poor contact between the PVK and electrode, which increases device series resistance and reduces short-circuit current density (J SC) and fill factor (FF). [21] To minimize the bulk and interfacial defects associated with inorganic PVKs, a variety of passivation strategies have been used, [21-28] including additive engineering and post-treatment. Nevertheless, most strategies focus on the passivation of either bulk or interfacial defects rather than both. On the other hand, considerable efforts have been devoted to maximizing the built-in electric field (BEF) of PeSCs, which facilitates carrier separation/transport and hence contributes to the V OC of the device. As the BEF is primarily determined by the work function difference between the two electrodes or transport layers (i.e., electron transport layer [ETL] and hole transport layer [HTL]), [29] BEF enhancement still remains