Unearthing Superior Inorganic UV Second‐Order Nonlinear Optical Materials: A Mineral‐Inspired Method Integrating First‐Principles High‐Throughput Screening and Crystal Engineering

(0.005@546 nm). Our research has not only revitalized the potential of the fresnoite mineral for the development of new high-performance UV nonlinear optical materials but has also provided a clearly defined roadmap for the efficient exploration of novel structure-driven functional materials with targeted properties.