This study investigates the functional neuroanatomy of harmonic music perception with fMRI. We presented short pieces of Western classical music to nonmusicians. The ending of each piece was systematically manipulated in the following four ways: Standard Cadence (expected resolution), Deceptive Cadence (moderate deviation from expectation), Modulated Cadence (strong deviation from expectation but remaining within the harmonic structure of Western tonal music), and Atonal Cadence (strongest deviation from expectation by leaving the harmonic structure of Western tonal music). Music compared with baseline broadly recruited regions of the bilateral superior temporal gyrus (STG) and the right inferior frontal gyrus (IFG). Parametric regressors scaled to the degree of deviation from harmonic expectancy identified regions sensitive to expectancy violation. Areas within the BG were significantly modulated by expectancy violation, indicating a previously unappreciated role in harmonic processing. Expectancy violation also recruited bilateral cortical regions in the IFG and anterior STG, previously associated with syntactic processing in other domains. The posterior STG was not significantly modulated by expectancy. Granger causality mapping found functional connectivity between IFG, anterior STG, posterior STG, and the BG during music perception. Our results imply the IFG, anterior STG, and the BG are recruited for higher-order harmonic processing, whereas the posterior STG is recruited for basic pitch and melodic processing.