Brain, as a complex cognitive system, often processes multiple dimension information synchronously and integrate them to adapt dynamic environments and make effective decisions.1-3 How to retrieve latent neurobehavioral processes from complex human neurobiological signals is an important yet previously unresolved challenge.4,5 For instance, the previous literature has proposed two fundamental yet mutually confounded processes during the decision making and affective processing, i.e. valance and arousal.6,7 Here, we develop a novel analytical approach, orthogonal-Decoding multi-Cognitive Processes (DeCoP), with which we dissociate neural responses in processing valence and arousal information during tests of motivational and emotional function. During reward/punishment anticipation, we decode brain-wide responses into spatially overlapping, yet functionally independent, evaluation and readiness networks, i.e., motivational valence and arousal processing, which are modulated differentially by the meso-limbic vs nigro-striatal dopamine systems. Similarly, during emotional reactivity, we decompose amygdala response into independent emotional valence and facial arousal processing features. We demonstrate that DeCoP can resolve paradoxically unexpected brain 'inactivation', and be applied more generally to decode multiple latent neurobehavioral processes. Furthermore, we anticipate our approach to advance both the design and hypothesis testing of cognitive experimental task paradigms.