Oxychalcogenides capable of exhibiting excellent balance among large second-harmonic generation (SHG) response, wide band gap (Eg ), and suitable birefringence (Δn) are ideal materials class for infrared nonlinear optical (IR NLO) crystals. However, rationally designing a new high-performance oxychalcogenide IR NLO crystal still faces a huge challenge because it requires the optimal orientations of the heteroanionic groups in oxychalcogenide. Herein, a series of antiperovskite-type oxychalcogenides, Ae3 Q[GeOQ3 ] (Ae = Ba, Sr; Q = S, Se), which were synthesized by employing the antiperovskite-type Ba3 S[GeS4 ] as the structure template. Their structures feature novel three-dimensinoal frameworks constructed by distorted [QAe6 ] octahedra, which are further filled by [GeOQ3 ] tetrahedra to form antiperovskite-type structures. Based on the unique antiperovskite-type structures, the favorable alignment of the polarizable [GeOQ3 ] tetrahedra and distorted [QAe6 ] octahedra have been achieved. These contribute the ideal combination of large SHG response (0.7-1.5 times that of AgGaS2 ), wide Eg (3.52-4.10eV), and appropriate Δn (0.017-0.035) in Ae3 Q[GeOQ3 ]. Theoretical calculations and crystal structure analyses revealed that the strong SHG and wide Eg could be attributed to the polarizable [GeOQ3 ] tetrahedra and distorted [QAe6 ] octahedra. This research provides a new exemplification for the design of high-performance IR NLO materials.