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We have derived new detailed abundances of Mg, Ca, and the Fe-group elements Sc through Zn ( Z = 21−30) for 37 main-sequence turnoff very metal-poor stars ([Fe/H] ≲−2.1). We analyzed Keck HIRES optical and near-UV high signal-to-noise spectra originally gathered for a Be abundance survey. Using typically ∼400 Fe-group lines with accurate laboratory transition probabilities for each star, we have determined accurate LTE metallicities and abundance ratios for neutral and ionized species of the 10 Fe-group elements as well as α elements Mg and Ca. We find good neutral/ion abundance agreement for the six elements that have detectable transitions of both species in our stars in the 3100–5800 Å range. Earlier reports of correlated Sc−Ti−V relative overabundances are confirmed, and appear to slowly increase with decreasing metallicity. To this element trio we add Zn; it also appears to be increasingly overabundant in the lowest-metallicity regimes. Co appears to mimic the behavior of Zn, but issues surrounding its abundance reliability cloud its interpretation.