Lateralization in the desynchronization of anticipatory occipitoparietal alpha (8-12 Hz) oscillations has been implicated in the allocation of selective visuospatial attention. Previous studies have demonstrated that small changes in the lateralization of alpha-band activity are predictive of behavioral performance but have not directly investigated how flexibly alpha lateralization is linked to top-down attentional goals. To address this question, we presented participants with cues providing varying degrees of spatial certainty about the location at which a target would appear. Time-frequency analysis of EEG data demonstrated that manipulating spatial certainty led to graded changes in the extent to which alpha oscillations were lateralized over the occipitoparietal cortex during the cue-target interval. We found that individual differences in alpha desynchronization contralateral to attention predicted reaction times, event-related potential measures of perceptual processing of targets, and beta-band (15-25 Hz) activity typically associated with response preparation. These results support the hypothesis that anticipatory alpha modulation is a plausible neural mechanism underlying the allocation of visuospatial attention and is under flexible top-down control.