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Brain-computer interfaces (BCIs) may be a future communication channel for motor-disabled people. In surface electroencephalogram (EEG)-based BCIs, the extracted features are often derived from spectral estimates and autoregressive models. We examined the usefulness of synchronization between EEG signals for classifying mental tasks. To this end, we investigated the performance of features derived from the phase locking value (PLV) and from the spectral coherence and compared them to the classification rates resulting from the power densities in α, β1, β2, and 8-30-Hz frequency bands. Five recordings of 60 min, acquired from three subjects while performing three different mental tasks, were analyzed offline. No artifacts were removed or rejected. We noticed significant differences between PLV and mean spectral coherence. For sole use of synchronization measures, classification accuracies up to 62% were achieved. In general, the best result was obtained combining phase synchronization measures with α power spectral density estimates. The results demonstrate that phase synchronization provides relevant information for the classification of spontaneous EEG during mental tasks.