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Fang and co‐workers report a non‐interpenetrated three‐dimensional covalent organic framework (JUC‐643) constructed from an 8‐connected building unit via a symmetry‐lowering design strategy. The framework features an unusual [4+3(+2)] connectivity and a jca topology, which effectively suppress the interpenetration commonly observed in 3D COFs. Benefiting from its open pore architecture, the material exhibits a high surface area, excellent structural stability, and enhanced adsorption performance toward light hydrocarbons, highlighting the effectiveness of symmetry lowering in the rational construction of non‐interpenetrated 3D COFs. Further details can be found in the article by Song et al . on pages 643—648. image