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To discover the nonlinear optical (NLO) materials with strong second harmonic generation (SHG), the design of NLO-active molecular units with large polarization is considered as a common strategy. Herein, we propose that the local structural distortion induced with vacancies, apart from the NLO-active units, can be employed to improve the NLO effect in solids as well. Accordingly, a new tungsten bronze (T oxide, Pb2(Pb0.15Li0.7□0.15)Nb5O15 (□ representing vacancies), is successfully designed and prepared, which exhibits a strong SHG re