With ever increasing demands to multitask, it has become particularly important to identify characteristics of (un)successful multitaskers. This chapter presents a review of a research program aimed at examining the role the need for cognitive closure (NFC)– a motivational tendency to reduce uncertainty, confusion, and ambiguity–plays in multitasking performance, preference, and behavior. In several lines of research (13 studies in total), we have found that high NFC individuals, in striving for more structure and order in their lives, preferred multitasking less and tended to engage in it to a lesser extent than low NFC individuals did. This, however, was only the case when multitasking was not required by the task rules. When multitasking was explicitly required, it was high, rather than low, NFC individuals who engaged in multitasking to a greater extent (despite their personal preference) and performed better in certain circumstances. Notably, high NFC individuals performed worse on concurrent tasks when they also had low shifting ability. However, when their shifting ability was high or given tasks were presented in the presence of task-irrelevant interruptions, high NFC individuals performed better than low NFC individuals did. Such effects were obtained due to the greater effort (indexed behaviorally or as cardiovascular reactivity) mobilized by high NFC individuals in order to comply with the task demands. Greater effort also compensated for the differences in attention between high and low NFC individuals (demonstrated in two separate eye-tracking studies). The collected results present the multifaceted nature of the tested relationship and add significantly to the literature on individual difference predictors of multitasking.