We present results from an observing campaign to identify low-metallicity stars in the Best & Brightest Survey. From medium-resolution (R~1200-2000) spectroscopy of 857 candidates, we estimate the stellar atmospheric parameters (T_eff_, logg, and [Fe/H]), as well as carbon and {alpha}-element abundances. We find that 69% of the observed stars have [Fe/H]<=-1.0, 39% have [Fe/H]<=-2.0, and 2% have [Fe/H]<=-3.0. There are also 133 carbon-enhanced metal-poor (CEMP) stars in this sample, with 97 CEMP Group I and 36 CEMP Group II stars identified in the A(C) versus [Fe/H] diagram. A subset of the confirmed low-metallicity stars were followed-up with high-resolution spectroscopy, as part of the R-process Alliance, with the goal of identifying new highly and moderately r-process-enhanced stars. Comparison between the stellar atmospheric parameters estimated in this work and from high-resolution spectroscopy exhibit good agreement, confirming our expectation that medium-resolution observing campaigns are an effective way of selecting interesting stars for further, more targeted, efforts.