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We report a series of Pd(II)nL2n coordination rings for which nuclearity is controlled by the binding angle of the corresponding bis‐monodentate bridging ligands. Judicious choice of the angle within a family of rather rigid ligands allowed for the first‐time to synthesize a homoleptic five‐membered Pd5L10 ring that does not require any template to form. We demonstrate that control over the ring size...