The synthesis of two 3D M2L4 copper(II) capsules, {[BF4⊂(CH3CN)2Cu2(L1)4][BF4]3} (1) and {[BF4⊂(BF4)2Cu2(L1)4][BF4]} (2), by using 1,3‐(benzimidazol‐1‐ylmethyl)‐2,5‐dimethoxy‐4,6‐dimethylbenzene (L1) as a semirigid exobidentate ligand and [Cu(CH3CN)4][BF4]2 as a metallobrick is reported. Single‐crystal X‐ray diffraction studies show the encapsulation of a BF4– anion in 1 and 2. Moreover, 2 displayed three coordinated BF4– anions, which is rare in supramolecular coordination host–guest chemistry. Remarkably, in both metallocages the weakly coordinated BF4– anion acts as a template and interacts with the metal center through a weak Cu···F contact. (© Wiley‐VCH Verlag GmbH & Co. KGaA, 69451 Weinheim, Germany, 2009)