To gain insight into four highly ionized high-velocity clouds (HVCs) discovered by Sembach et al. (1999), we have analyzed data from the Hubble Space Telescope (HST) and Far Ultraviolet Spectroscopic Explorer (FUSE) for the PKS 2155-304 and Mrk 509 sight lines. We measure strong absorption in OVI and column densities of multiple ionization stages of silicon (SiII/III/IV) and carbon (CII/III/IV). We interpret this ionization pattern as a multiphase medium that contains both collisionally ionized

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... and photoionized gas. Toward PKS 2155-304, for HVCs at -140 and -270 km/s, respectively, we measure logN(OVI)=13.80+/-0.03 and log N(OVI)=13.56+/-0.06; from Lyman series absorption, we find log N(HI)=16.37^(+0.22)_(-0.14) and 15.23^(+0.38)_(-0.22). The presence of high-velocity OVI spread over a broad (100 km/s) profile, together with large amounts of low-ionization species, is difficult to reconcile with the low densities, n=5x10^(-6) cm^(-3), in the collisional/photoionization models of Nicastro et al. (2002), although the HVCs show a similar relation in N(SiIV)/N(CIV) versus N(CII)/N(CIV) as high-z intergalactic clouds. Our results suggest that the high-velocity OVI in these absorbers do not necessarily trace the WHIM, but instead may trace HVCs with low total hydrogen column density. We propose that the broad high-velocity OVI absorption arises from shock ionization, at bowshock interfaces produced from infalling clumps of gas with velocity shear. The similar ratios of high ions for HVC Complex C and these highly ionized HVCs suggest a common production mechanism in the Galactic halo.