Dual tasks (DTs) require additional control processes that temporally coordinate the processing of the two component tasks. Previous studies employing imaging as well as noninvasive stimulation techniques have demonstrated that the dorsolateral prefrontal cortex (dlPFC) is causally involved in these task-order coordination processes. However, in these studies, participants were instructed to match their processing order to an externally provided and mandatory order criterion during DT processing. Hence, it is still unknown whether the dlPFC is also recruited for rather voluntary order control processes, which are required in situations that allow for intentional and internally generated order choices. To address this issue, in two experiments, we applied anodal (Experiment 1) and cathodal (Experiment 2) transcranial direct current stimulation during a random-order DT in which participants could freely decide about their order of task processing. In our results, we found facilitatory and inhibitory effects on voluntary task-order coordination because of anodal and cathodal transcranial direct current stimulation, respectively. This was indicated by shorter RTs when participants intentionally switched the task order relative to the preceding trial during anodal as well as a reduced tendency to switch the task order relative to the preceding trial during cathodal stimulation compared with the sham stimulation. Overall, these findings indicate that the dlPFC is also causally involved in voluntary task-order coordination processes. In particular, we argue that the dlPFC is recruited for intentionally updating and implementing task-order information that is necessary for scheduling the processing of two temporally overlapping tasks.