Dual tasks are characterized by the requirement for additional task-order coordination processes that schedule the processing order of two temporally overlapping tasks. Preliminary evidence from functional imaging studies suggests that lateral pFC (lPFC) activation correlates with implementing these task-order coordination processes. However, so far, it is unclear whether the lPFC is also causally involved in coordinating task order during dual-task performance and which exact mechanisms are implemented by this brain region. In this study, we addressed these open issues by applying online TMS during a dual-task situation. For this purpose, participants performed a dual task in fixed-order blocks with a constant order of tasks and in random-order block, in which the order of tasks varied randomly and thus demands on task-order coordination were increased. In Experiment 1, TMS of the lPFC compared with control TMS conditions impaired dual-task performance in random-order blocks, whereas performance in fixed-order blocks was unaffected by TMS. In Experiment 2, we tested for the specificity of the lPFC TMS effect on task-order coordination by applying TMS over the preSMA. We showed that preSMA TMS did not affect dual-task performance, neither in fixed-order nor in random-order blocks. Results of this study indicate that the lPFC, but not the preSMA, is causally involved in implementing task-order coordination processes in dual-task situations.