Recent neurocognitive models propose that the insula serves as a hub of interoceptive awareness system, modulating 2 interplaying neurocognitive systems: The posterior insula (PI) receives and integrates various interoceptive signals; these signals are then transmitted to the anterior insula for processing higher-order representations into awareness, where the dorsal anterior insula (dAI) modulates the prefrontal self-control system and the ventral anterior insula (vAI) modulates the amygdala (AMG)-striatal reward-seeking circuit. We sought to test this view using a multimodal approach. We first used a resting-state functional magnetic resonance imaging (fMRI) approach with a sample of 120 undergraduate students. Then, we unpacked the neuro-cognitive association between insular connectivity and cognitive performance during an Iowa gambling fMRI task. Lastly, an independent Open Southwest University Longitudinal Imaging Multimodal dataset was used to validate the results. Findings suggested that the dAI was predominantly connected to the prefrontal regions; the vAI was primarily connected to the AMG–ventral–striatum system; and the PI was mainly connected to the visceral-sensorimotor system. Moreover, cognitive scores were positively correlated with FC between dAI and the self-control process of ventrolateral prefrontal cortex and were negatively correlated with FC between vAI and the reward-seeking process of orbitofrontal cortex and subgenual anterior cingulate cortex. The findings highlight the roles of our theorized subinsular functionality in the overall operation of the neural cognitive systems.