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To introduce crown ethers into the struts of metal–organic frameworks (MOFs), general approaches have been developed for the syntheses of dicarboxylic acid dibenzo 30 crown‐10 (DB30C10DA), dicarboxylic acid di‐2, 3‐naphtho 30 crown‐10 (DN30C10DA), dicarboxylic acid bisparaphenylene 34 crown‐10 (BPP34C10DA), and dicarboxylic acid 1, 5‐naphthoparaphenylene 36 crown‐10 (NPP36C10DA). These novel crown ethers not only retain the characteristics of their parent crown ethers since they can 1) bind cationic guests and 2) serve as templates for making mechanically interlocked molecules (MIMs), such as catenanes and rotaxanes, but they also present coordination sites to connect with secondary building units (SBUs) in MOFs. The binding behavior of BPP34C10DA with 1, 1′‐dimethyl‐4, 4′‐bipyridinium bis (hexafluorophosphate)(DMBP⋅ 2 PF6) has been investigated by means of UV/Vis …