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Nonlinear optical (NLO) crystals are widely applied in information technology, micro‐manufacturing and medical treatment. Herein, a new lead mixed halide with strong second‐harmonic generation (SHG) response, Cs3Pb2(CH3COO)2Br3I2, has been designed and rationally synthesized. Cs3Pb2(CH3COO)2Br3I2 represents the rare NLO crystal featuring that three different anions (I−, Br− and O2−) simultaneously...