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Neurofeedback cognitive training is a promising tool used to promote cognitive functions effectively and efficiently. In this study, we investigated a novel functional near-infrared spectroscopy (fNIRS)-based frontoparietal functional connectivity (FC) neurofeedback training paradigm related to working memory, involving healthy adults. Compared with conventional cognitive training studies, we chose the frontoparietal network, a key brain region for cognitive function modulation, as neurofeedback, yielding a strong targeting effect. In the experiment, 10 participants (test group) received three cognitive training sessions of 15 min using fNIRS-based frontoparietal FC as neurofeedback, and another 10 participants served as the control group. Frontoparietal FC was significantly increased in the test group ( $p =0.03$ ), and the cognitive functions (memory and attention) were significantly promoted compared with the control group (accuracy of 3-back test: $p =0.0005$ , reaction time of 3-back test: $p =0.0009$ ). After additional validations on long-term training effect and on different patient populations, the proposed method exhibited considerable potential to be developed as a fast, effective, and widespread training approach for cognitive function enhancement.