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Heart rate variability biofeedback (HRV-BF) has been confirmed to increase heart rate variability (HRV) and cardiac outflows by baroreflex in healthy populations and clinical patients. Autogenic training (AT) is common used in the psychological intervention. This study integrates a single-session of HRV-BF and AT into a high-technology mobile application (app), and examines the effects on HRV indices, breathing rates, and subjective relaxation scores. Healthy college students were recruited and assigned to the single-session HRV-BF group or AT group. Participants in the HRV-BF group received HRV-BF combined with paced breathing training, which gradually stepped down their breathing rates from 12, to 8, to 6 breaths/per min; and received feedback of HRV indices from the app. Participants in the AT group received autogenic training and feedback of heart rate from the app. A chest belt Zephyr BioHarness was connected through Bluetooth to a Zenfone5 mobile phone, it collected the signals of interbeat intervals and breathing rates at pre-training, mid-training, and post-training stages. The Kubios HRV software was used to analyze HRV indices. The results reveal higher HRV indices and lower breathing rates during mid-training and post-training in the HRV-BF group compared to the AT group. There were higher high-frequency of HRV at post-training than pre-training in the AT group. Participants of both groups increased their subjective relaxation scores after training. The HRV-BF protocol increased cardiac outflows by baroreflex and decreased breathing rates, and the AT protocol increased high-frequency of HRV. These high-technology wearable devices combined with psychological interventions will apply to various populations in the future.