We present measurements of [Fe/H] and [{alpha}/Fe] for 128 individual red giant branch stars (RGB) in the stellar halo of M31, including its Giant Stellar Stream (GSS), obtained using spectral synthesis of low- and medium-resolution Keck/DEIMOS spectroscopy (R~3000 and 6000, respectively). We observed four fields in M31's stellar halo (at projected radii of 9, 18, 23, and 31kpc), as well as two fields in the GSS (at 33kpc). In combination with existing literature measurements, we have increased the sample size of [Fe/H] and [{alpha}/Fe] measurements from 101 to a total of 229 individual M31 RGB stars. From this sample, we investigate the chemical abundance properties of M31's inner halo, finding <[Fe/H]>=-1.08+/-0.04 and <[{alpha}/Fe]>=0.40+/-0.03. Between 8 and 34kpc, the inner halo has a steep [Fe/H] gradient (-0.025+/-0.002dex/kpc) and negligible [{alpha}/Fe] gradient, where substructure in the inner halo is systematically more metal-rich than the smooth component of the halo at a given projected distance. Although the chemical abundances of the inner stellar halo are largely inconsistent with that of present-day dwarf spheroidal (dSph) satellite galaxies of M31, we identified 22 RGB stars kinematically associated with the smooth component of the stellar halo that have chemical abundance patterns similar to M31 dSphs. We discuss formation scenarios for M31's halo, concluding that these dSph-like stars may have been accreted from galaxies of similar stellar mass and star formation history, or of higher stellar mass and similar star formation efficiency.