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Coordination-directed synthesis has emerged as an effective and versatile approach for constructing mechanically interlocked molecules (MIMs). This field has long been dominated by Werner-type complexes featuring oxygen and/or nitrogen donors, whereas assemblies incorporating N-heterocyclic carbene (NHC) donors remain underexplored. This Review provides a comprehensive overview of the rapidly developing field of MIMs constructed from poly-NHC-based building blocks. By highlighting representative recent examples, this Review focuses on the pivotal role of NHC ligands and the robustness of the metal–CNHC bond in the construction of metallosupramolecular interlocked structures. In addition, this Review summarizes contemporary strategies for achieving efficient assembly, analyzes defining structural attributes of the resulting architectures, and outlines current challenges and emerging opportunities for future developments in NHC-based MIMs.