Reaction of hydrated Zn[NO3](2) or Zn[BF4](2) with four or more equivalents of 3{5}-tert-butylpyrazole (L-tBu) yields [Zn(L-tBu)(4)]X-2(X- = NO3- or BF4-). The nitrate complex contains C-2-symmetric four-coordinate zinc(II) centers with a slightly flattened tetrahedral geometry, and each nitrate anion hydrogen bonds to two pyrazole N-H groups. Similar reactions with Zn[ClO4](2) or ZnCl2 in the presence of 2 equiv of AgPF6 or AgSbF6 yield instead [{Zn(L-tBu)(4)}(L-tBu)(4)][ClO4](2) and [{Zn(L-tBu)(4)}(L-tBu)(2)]Y-2(Y-=PF6- or SbF6-). Crystals of [{Zn(L-tBu)(4)}(L-tBu)(4)][ClO4](2) are composed of discrete [{Zn(L-tBu)(4)}(L-tBu)(4)](2+) supramolecules that are formed from N-H...N hydrogen bonding between zinc-bound and uncoordinated pyrazole rings. The [{Zn(L-tBu)(4)}(L-tBu)(4)](2+) moieties are linked into planar 4(4) nets by hydrogen bonding to bridging ClO4- anions. The ClO4- ions are almost perfectly encapsulated in near-spherical cavities of approximate dimensions 5.0 x 5.0 x 4.5 angstrom that are formed by two interlocked supramolecular dications. Similarly, [{Zn(L-tBu)(4)}(L-tBu)(2)][PF6](2) crystallizes as discrete supramolecules in the crystal with the PF(6)(-)anions occupying a shallow bowl-shaped cavity on the surface of the complex that is formed by two zinc-bound and one uncoordinated pyrazole ligands. H-1 NMR and IR studies of [{Zn(L-tBu)(4)}(L-tBu)(4)][ClO4](2) in CD2Cl2 imply that the second-sphere LtBu ligands dissociate from the [Zn(L-tBu)(4)](2+) center in this solvent and that free and metal-bound LtBu are in rapid chemical exchange.