Emotion regulation plays a key role in human behavior and overall well-being. Neurofeedback is a non-invasive self-brain training technique used for emotion regulation to enhance brain function and treatment of mental disorders through behavioral changes. Previous neurofeedback research often focused on using activity from a single brain region as measured by fMRI or power from one or two EEG electrodes. In a new study, we employed connectivity-based EEG neurofeedback through recalling positive autobiographical memories and simultaneous fMRI to upregulate positive emotion. In our novel approach, the feedback was determined by the coherence of EEG electrodes rather than the power of one or two electrodes. We compared the efficiency of this connectivity-based neurofeedback to traditional activity-based neurofeedback through multiple experiments. The results showed that connectivity-based neurofeedback effectively improved BOLD signal change and connectivity in key emotion regulation regions such as the amygdala, thalamus, and insula, and increased EEG frontal asymmetry, which is a biomarker for emotion regulation and treatment of mental disorders such as PTSD, anxiety, and depression and coherence among EEG channels. The psychometric evaluations conducted both before and after the neurofeedback experiments revealed that participants demonstrated improvements in enhancing positive emotions and reducing negative emotions when utilizing connectivity-based neurofeedback, as compared to traditional activity-based and sham neurofeedback approaches. These findings suggest that connectivity-based neurofeedback may be a superior method for regulating emotions and could be a useful alternative therapy for mental disorders, providing individuals with greater control over their brain and mental functions.