Cobalt-59 NMR spectra of stationary powder samples of salts containing Co(C2B9H11)(2)(-) and Co(C5H5)(2)(+) have been acquired at 21.14 T using single-echo stepped-frequency experiments. The resulting central transition, m(I) = 1/2 <-> m(I) = -1/2, line shapes span more than 2.0 MHz and are dominated by the second-order quadrupolar interaction. Analysis of the spectra leads to C-Q values of ca. 163 MHz for both ions, among the largest Co-59 C-Q values reported. In addition, Co-59 chemical shift anisotropies are significant for Co(C2B9H11)(2)(-) and Co(C5H5)(2)(+), with values of 4500-4700 and 5650 ppm, respectively. Isotropic Co-59 chemical shifts for the cobalticarborane anion are unavailable from NMR measurements of solution samples, probably because of the extremely short relaxation times anticipated for this complex.