Growing evidence of transcranial alternating current stimulation (tACS) modulating intrinsic neural oscillations has spawned interest in applying tACS to treat psychiatric disorders associated with aberrant neural oscillations. The alpha rhythmic activity is known to dominate neural oscillations at the awake, restful state, while attenuated resting-state alpha activity has been implicated in anxious mood. Administering repeated alpha-frequency tACS (α-tACS; at individual peak alpha frequency; 8-12 Hz) over four consecutive days (in the experiment group, sham stimulation in the control group), we demonstrated immediate and lasting (>24 h) increases in resting-state posterior ➔frontal connectivity in the alpha frequency, quantified by Granger causality. Critically, this connectivity enhancement was accompanied by sustained reductions in both anxious arousal and negative perception of sensory stimuli. Resting-state alpha power also increased, albeit only transiently, reversing to the baseline level within 24 h after tACS. Therefore, the lasting enhancement of long-range alpha connectivity due to α-tACS differs from local alpha activity that is nonetheless conserved, highlighting the adaptability of alpha oscillatory networks. In light of increasing recognition of large-scale network dysfunctions as a transdiagnostic pathophysiology of psychiatric disorders, this enduring connectivity plasticity, along with the behavioral improvements, paves the way for tACS applications in clinical interventions of psychiatric 'oscillopathies'.