Electroencephalography (EEG) connectomes offer powerful tools for studying brain connectivity and advancing our understanding of brain function and dysfunction in both healthy and pathological conditions. Celebrating the 100th anniversary of EEG discovery, this Perspective explores the frontiers of EEG-based brain connectivity in basic and translational neuroscience research. We review new concepts, emerging analysis frameworks and significant advances in harnessing EEG connectomes. We suggest that leveraging machine learning approaches may offer promising paths to maximize the strengths of EEG connectomes. We also discuss how combined EEG connectome and neuromodulation provide a personalized and adaptive closed-loop paradigm to promote neuroplasticity and treat dysfunctional brains. We further address the limitations and challenges of the current methodology and touch on important issues regarding research rigour and clinical viability for translational impact.