Continued human and animal research has strengthened evidence for aberrant excitatory–inhibitory neural processes underlying autism and schizophrenia spectrum disorder psychopathology, particularly psychosocial functioning, in clinical and nonclinical populations. We investigated the extent to which autistic traits and schizotypal dimensions were modulated by the interactive relationship between excitatory glutamate and inhibitory GABA neurotransmitter concentrations in the social processing area of the superior temporal cortex using proton magnetic resonance spectroscopy. In total, 38 non-clinical participants (20 females; age range = 18–35 years, mean (standard deviation) = 23.22 (5.52)) completed the autism spectrum quotient and schizotypal personality questionnaire, and underwent proton magnetic resonance spectroscopy to quantify glutamate and GABA concentrations in the right and left superior temporal cortex. Regression analyses revealed that glutamate and GABA interactively modulated autistic social skills and schizotypal interpersonal features ( pcorr < 0.05), such that those with high right superior temporal cortex glutamate but low GABA concentrations exhibited poorer social and interpersonal skills. These findings evidence an excitation–inhibition imbalance that is specific to psychosocial features across the autism and schizophrenia spectra.