The ability to adjust our behavior flexibly depending on situational demands and changes in the environment is an important characteristic of cognitive control. Previous studies have proved that this type of adaptive control plays a crucial role in selective attention, but have barely explored whether and how attentional networks support adaptive control. In the present study, a Stroop task with a different proportion of incongruent trials was used to investigate the brain activity and connectivity of six typical attentional control networks (i.e., the fronto-parietal network (FPN), cingulo-opercular network (CON), default mode network (DMN), dorsal attention network (DAN), and ventral attention network/salience network (VAN/SN)) in the environment with changing control demand. The behavioral analysis indicated a decreased Stroop interference (incongruent vs. congruent trial response time [RT]) with the increase in the proportion of incongruent trials within a block, indicating that cognitive control was improved there. The fMRI data revealed that the attenuate Stroop interference was accompanied by the activation of frontal and parietal regions, such as bilateral dorsolateral prefrontal cortex and anterior cingulate cortex. Crucially, the improved cognitive control induced by the increased proportion of incongruent trials was associated with the enhanced functional connectivity within the five networks, and a greater connection between CON with the DAN/SN, and between DMN with the CON/DAN/SN. Meanwhile, however, the functional coupling between the FPN and VAN was decreased. These results suggest that flexible regulations of cognitive control are implemented by the large-scale reconfiguration of connectivity patterns among the attentional networks.