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The activities of the brain and the heart are dynamic, chaotic, and possibly intrinsically coordinated. This study aims to investigate the effect of Mindfulness-Based Stress Reduction (MBSR) program on the chaoticity of electronic activities of the brain and the heart, and to explore their potential correlation. Electroencephalogram (EEG) and electrocardiogram (ECG) were recorded at the beginning of an 8-week standard MBSR training course and after the course. EEG spectrum analysis was carried out, wavelet entropies (WE) of EEG (together with reconstructed cortical sources) and heart rate were calculated, and their correlation was investigated. We found enhancement of EEG power of alpha and beta waves and lowering of delta waves power during MBSR training state as compared to normal resting state. Wavelet entropy analysis indicated that MBSR mindfulness meditation could reduce the chaotic activities of both EEG and heart rate as a change of state. However, longitudinal change of trait may need more long-term training. For the first time, our data demonstrated that the chaotic activities of the brain and the heart became more coordinated during MBSR training, suggesting that mindfulness training may increase the entrainment between mind and body. The 3D brain regions involved in the change in mental states were identified.