The low-frequency (<0.1 Hz) fluctuation in sustained attention attracts enormous interest in cognitive neuroscience and clinical research since it always leads to cognitive and behavioral lapses. What is the source of the spontaneous fluctuation in sustained attention in neural activity, and how does the neural fluctuation relate to behavioral fluctuation? Here, we address these questions by collecting and analyzing two independent fMRI and behavior datasets. We show that the neural (fMRI) fluctuation in a key brain network, the default-mode network (DMN), mediate behavioral (reaction time) fluctuation during sustained attention. DMN shows the increased amplitude of fluctuation, which correlates with the behavioral fluctuation in a similar frequency range (0.01-0.1 Hz) but not in the lower (<0.01 Hz) or higher (>0.1 Hz) frequency range. This was observed during both auditory and visual sustained attention and was replicable across independent datasets. These results provide a novel insight into the neural source of attention-fluctuation and extend the former concept that DMN was deactivated in cognitive tasks. More generally, our findings highlight the temporal dynamic of the brain-behavior relationship.