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The rational control of intrinsic defects in materials can significantly enhance their scientific and technological potentials, but it remains a long‐standing challenge in nanocrystal‐in‐glass composites (NGCs). Herein, a defect engineering strategy mediated by the mixed alkali effect is proposed and experimentally demonstrated for NGCs. Interestingly, the hybridization of large alkali ions can effectively increase the barrier of Li+ migration and reduce the Li‐related defects in LiNbO3 NGC. As a result, a novel LiNbO3 NGC with greatly reduced Li‐related defects, high crystallinity of over 60%, and excellent optical transmission are successfully fabricated. This unique NGC configuration facilitates efficient transverse second harmonic generation (TSHG) in a broad wavelength region. Based on the above effects, a standard TSHG device is fabricated and implemented to monitor ultrashort optical pulses with duration in the order of ≈10−13 s over a broad wavelength region, down to 780 nm. The proposed strategy not only provides a new idea for defect engineering in materials science but also has great significance for boosting the practical applications of NGCs in ultrashort optical pulse monitoring. [ABSTRACT FROM AUTHOR]