We describe an ambitious ongoing study that has been strongly influenced and inspired by Don Stuss's career-long efforts to identify key cognitive processes that characterize executive control, investigate potential unifying dimensions that define prefrontal function, and carefully attend to individual differences. The Dual Mechanisms of Cognitive Control project tests a theoretical framework positing two key control dimensions: proactive and reactive. The framework's central tenets are that proactive and reactive control modes reflect domain-general dimensions of individual variation, with distinctive neural signatures, involving the lateral pFC as a central node within associated brain networks (e.g., fronto-parietal, cingulo-opercular). In the Dual Mechanisms of Cognitive Control project, each participant is scanned while performing theoretically targeted variants of multiple well-established cognitive control tasks (Stroop, cued task-switching, AX-CPT, Sternberg working memory) in three separate imaging sessions, that each encourages utilization of different control modes plus also completes an extensive out-of-scanner individual differences battery. Additional key features of the project include a high spatio-temporal resolution (multiband) acquisition protocol and a sample that includes a substantial subset of monozygotic twin pairs and participants recruited from the Human Connectome Project. Although data collection is still continuing (target n = 200), we provide an overview of the study design and protocol, along with initial results (n = 80) revealing evidence of a domain-general neural signature of cognitive control and its modulation under reactive conditions. Aligned with Don Stuss's legacy of scientific community building, a partial data set has been publicly released, with the full data set released at project completion, so it can serve as a valuable resource. © 2021 Massachusetts Institute of Technology.