Although there have been major strides toward uncovering the neurobehavioral mechanisms involved in cognitive functions like memory and decision making, methods for measuring behavior and accessing latent processes through computational means remain limited. To this end, we have created SUPREME (Sensing to Understanding and Prediction Realized via an Experiment and Modeling Ecosystem): a toolbox for comprehensive cognitive assessment, provided by a combination of construct-targeted tasks and corresponding computational models. SUPREME includes four tasks, each developed symbiotically with a mechanistic model, which together provide quantified assessments of perception, cognitive control, declarative memory, reward valuation, and frustrative nonreward. In this study, we provide validation analyses for each task using two sessions of data from a cohort of cognitively normal participants (N = 65). Measures of test-retest reliability (r: 0.58–0.75), stability of individual differences (ρ: 0.56–0.70), and internal consistency (α: 0.80–0.86) support the validity of our tasks. After fitting the models to data from individual subjects, we demonstrate each model’s ability to capture observed patterns of behavioral results across task conditions. Our computational approaches allow us to decompose behavior into cognitively interpretable subprocesses, which we can compare both within and between participants. We discuss potential future applications of SUPREME, including clinical assessments, longitudinal tracking of cognitive functions, and insight into compensatory mechanisms.