Although motor coordination and imitation are important factors affecting motor skill learning, few studies have examined the relationship between them in healthy adults. In order to address this in the present study, we used fNIRS to analyze the relationship between motor coordination and imitation in college students. Our results showed that: (1) motor coordination in female students was positively correlated with the average time taken to perform an imitation; (2) the mean imitation time was negatively correlated with the activation level of the supplementary motor cortex, primary somatosensory cortex, and angular gyrus of the mirror neuron system; (3) motor coordination in female students moderated mirror neuron system (MNS) activation and imitation. For women with low rather than high motor coordination, higher MNS activation was associated with a stronger imitation ability. These results demonstrate that motor coordination in female students is closely related to action imitation, and that it moderates the activation of the MNS, as measured via fNIRS.