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Utilization of well‐defined siloxane molecules allows for the construction of functional siloxane‐based nanoporous materials based on the molecular design. Herein, a novel class of siloxane‐based porous materials is synthesized via cross‐linking of dimethylsilyl‐ and dimethylvinylsilyl‐functionalized cage siloxanes with double‐6‐ring (D6R) geometry. Compared with the conventional double‐4‐ring cage...