Solid-state double-resonance and triple-resonance C-13, B-11, and H-1 NMR experiments are used to investigate two main group metallocene complexes: the decamethylcyclopentadienylborinium cation, [C-P*B-2](+), and bis(pentamethylcyclopentadienyl)methylborane, C-P*2BMe. The crystal structure for the latter complex is reported herein. A combination of magic-angle-spinning and static B-11{H-1} NMR experiments are used to measure B-11 nuclear quadrupole coupling constants (C-Q) and rare instances of anisotropic boron chemical shielding tensors. Boron-11 nuclear quadrupole coupling constants reflect the higher spherical symmetry of [C-P*B-2](+) compared to C-P*2BMe, with C-Q(B-11) = 1.14 MHz in the former and C-Q(B-11) = 4.52 MHz in the latter. Chemical shielding tensor spans are measured for [C-P*B-2](+) and C-P*2BMe as Omega = 73.0 and 146.0 ppm, respectively. Hartree-Fock and hybrid density functional theory (B3LYP) calculations of electric field gradient and chemical shielding tensors are in quantitative agreement with experiment, and are applied to examine the relationships between the anisotropic NMR interaction tensors and the structure and symmetry of these chemically analogous but structurally dissimilar boron complexes. Variable-temperature B-11 MAS NMR, C-13 CPMAS NMR, and C-13/B-11/H-1 CP TRAPDOR NMR experiments are applied to make a preliminary investigation of motion of the C-P* rings Of [C-P*B-2](+).