Multiple Nd isotopic analyses were obtained for one metaluminous and two peralkaline Tertiary rhyolitic ash-flow tuffs in the Great Basin to determine whether upper crustal silicic magmas chemically evolve under closed- or open-system conditions. All the ash-flow tuffs analyzed show significant internal Nd isotopic variations. The largest variations occur within the peralkaline Double-H Mountains Tuff (ϵNd= +2.0 to +6.4) at the McDermitt volcanic field in north-central Nevada, and the smallest within the metaluminous Topopah Spring Tuff (ϵNd = -10.6 to -11.7) at the southwestern Nevada volcanic field. In all cases the isotopic variations are correlated with magmatic Nd contents, even though the Nd concentrations decreased roofward for the metaluminous rhyolite and increased for the peralkaline rhyolites. The consistent positive correlation between [Nd] and ϵNd provides strong evidence for in situ open-system addition of low ϵNd wall-rock material to the silicic magmas during their residence in the upper crust. The proportion of wall-rock Nd required to produce the isotopic zonations is small (1 to 15 mol%) for both the peralkaline and metaluminous rhyolites. All levels of the parental magmas sampled by the ash-flow tuffs, and not just magma occupying the roof zone, were open to wall-rock interaction. These results suggest that upper crystal silicic magma bodies evolve under open-system conditions and the effects of such processes should be addressed in models for their chemical differentiation.