We have conducted a radar-driven observational campaign of 22 main-belt asteroids (MBAs) focused on Bus–DeMeo Xc- and Xk-type objects (Tholen X and M class asteroids) using the Arecibo radar and NASA Infrared Telescope Facilities (IRTF). Sixteen of our targets were near-simultaneously observed with radar and those observations are described in a companion paper (Shepard, M.K., and 19 colleagues [2010]. Icarus, in press). We find that most of the highest metal-content asteroids, as suggested by radar, tend to exhibit silicate absorption features at both 0.9 and 1.9 μm, and the lowest metal-content asteroids tend to exhibit either no bands or only the 0.9 μm band. Eleven of the asteroids were observed at several rotational longitudes in the near-infrared and significant variations in continuum slope were found for nine in the spectral regions 1.1–1.45 μm and 1.6–2.3 μm. We utilized visible wavelength data (Bus, S.J., Binzel, R.P. [2002b]. Icarus 158, 146–177; Fornasier, S., Clark, B.E., Dotto, E., Migliorini, A., Ockert-Bell, M., Barucci, M.A. [2010]. Icarus 210, 655–673.) for a more complete compositional analysis of our targets. Compositional evidence is derived from our target asteroid spectra using two different methods: (1) a χ 2 search for spectral matches in the RELAB database, and (2) parametric comparisons with meteorites. This paper synthesizes the results of the RELAB search and the parametric comparisons with compositional suggestions based on radar observations. We find that for six of the seven asteroids with the highest iron abundances, our spectral results are consistent with the radar evidence (16 Psyche, 216 Kleopatra, 347 Pariana, 758 Mancunia, 779 Nina, and 785 Zwetana). Three of the seven asteroids with the lowest metal abundances, our spectral results are consistent with the radar evidence (21 Lutetia, 135 Hertha, 497 Iva). The remaining seven asteroids (22 Kalliope, 97 Klotho, 110 Lydia, 129 Antigone, 224 Oceana, 678 Fredegundis, and 771 Libera) have ambiguous compositional interpretations when comparing the spectral analogs to the radar analogs. The number of objects with ambiguous results from this multi-wavelength survey using visible, near-infrared, and radar wavelengths indicates that perhaps a third diagnostic wavelength region (such as the mid-infrared around 2–4 μm, the mid-infrared around 10–15 μm, and/or the ultraviolet around 0.2–0.4 μm) should be explored to resolve the discrepancies.