The present study investigated music-syntactic processing with chord sequences that ended on either regular or irregular chord functions. Sequences were composed such that perceived differences in the cognitive processing between syntactically regular and irregular chords could not be due to the sensory processing of acoustic factors like pitch repetition, pitch commonality (the major component of “sensory dissonance”), or roughness. Three experiments with independent groups of subjects were conducted: a behavioral experiment and two experiments using electroencephalography. Irregular chords elicited an early right anterior negativity (ERAN) in the event-related brain potentials (ERPs) under both task-relevant and task-irrelevant conditions. Behaviorally, participants detected around 75% of the irregular chords, indicating that these chords were only moderately salient. Nevertheless, the irregular chords reliably elicited clear ERP effects. Amateur musicians were slightly more sensitive to musical irregularities than nonmusicians, supporting previous studies demonstrating effects of musical training on music-syntactic processing. The findings indicate that the ERAN is an index of music-syntactic processing and that the ERAN can be elicited even when irregular chords are not detectable based on acoustical factors such as pitch repetition, sensory dissonance, or roughness.