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The interionic structure in solution of a series of [LAu(μ‐H)2WCp2][BF4] ion pairs (L=N‐heterocyclic carbene, phosphine or phosphite) has been elucidated by means of heteronuclear NOE and diffusion NMR. Selective ion pairing based on specific metallocene‐anion interactions has been observed for all species. The ancillary ligand L plays only a minor role in dictating the availability of secondary ion...