Abstract We present the first measurements of [Fe/H] and abundances, obtained using spectral synthesis modeling, for red giant branch stars in M31's giant stellar stream (GSS). The spectroscopic observations, obtained at a projected distance of 17 kpc from M31's center, yielded 61 stars with [Fe/H] measurements, including 21 stars with measurements, from 112 targets identified as M31 stars. The [Fe/H] measurements confirm the expectation from photometric metallicity estimates that stars in this region of M31's halo are relatively metal rich compared to stars in the Milky Way’s inner halo: more than half the stars in the field, including those not associated with kinematically identified substructure, have [Fe/H] abundances . The stars in this field are α-enhanced at lower metallicities, while decreases with increasing [Fe/H] above metallicities of [Fe/H] ≳ −0.9. Three kinematical components have been previously identified in this field: the GSS, a second kinematically cold feature of unknown origin, and M31's kinematically hot halo. We compare probabilistic [Fe/H] and distribution functions for each of the components. The GSS and the second kinematically cold feature have very similar abundance distributions, while the halo component is more metal poor. Although the current sample sizes are small, a comparison of the abundances of stars in the GSS field with abundances of M31 halo and dSph stars from the literature indicate that the progenitor of the stream was likely more massive, and experienced a higher efficiency of star formation, than M31's existing dSphs or the dEs NGC 147 and NGC 185.