Transcranial alternating current stimulation (tACS) at 10Hz influences spatial attention. However, the neural mechanisms by which tACS modulates spatial attention remain poorly understood. Here, we applied high-definition tACS at the individual alpha frequency (IAF), two control frequencies (IAF+/-2Hz) and sham to the left posterior parietal cortex and measured its effects on visuospatial attention performance as well as alpha power (using electroencephalography, EEG). Our results revealed a leftward lateralization of alpha power relative to sham. At a high value of leftward alpha lateralization, we also observed a leftward attention bias, which differed from sham. Moreover, the magnitude of the alpha lateralization effect predicted the attention bias. These effects occurred for tACS at IAF but not for the control frequencies. This suggests that tACS operates through oscillatory interactions with ongoing brain rhythms in line with synchronization theory. Our results also highlight the importance of personalized stimulation protocols, especially in potential clinical settings.