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Current CsPbBr 3 perovskite solar cells still suffer from a high open-circuit voltage (V oc ) loss due to the high defect density. Herein, we demonstrate a strategy to passivate defects and induce Fermi level modification through BaI 2 doping. The carrier lifetime is significantly extended after adding BaI 2 . In addition, the Fermi level is changed as Ba 2+ enters the crystal lattice, which increases the built-in potential and promotes the transport of carriers. As a result, the optimized thermally evaporated device shows a record V oc of 1.551 V and an improved power conversion efficiency of 10.09% as well as excellent thermal stability.

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