By means of transcranial direct current stimulation applied to the left dorsolateral prefrontal cortex, we investigated the causal role of increased or decreased excitability of this brain region for two facets of executive functions: working memory and Stroop interference control. We tested 1) whether anodal tDCS of the left DLPFC enhances working memory 15 minutes after termination of stimulation and in the absence of direct task practice under stimulation; 2) whether anodal tDCS of the left DLPFC enhances interference control, as evidenced by Stroop performance and Stroop sequence effects; and 3) whether cathodal tDCS leads to compromised executive functioning compared to anodal stimulation. In a between-subject design with 88 healthy psychology students, we compared the impact of anodal and cathodal stimulation against a sham condition, on performance on a Stroop task (during active stimulation) and on an n-back task (completed 15 minutes after active stimulation ended). We found significantly enhanced accuracy in the n-back task after anodal stimulation compared with sham, as well as speeded reactions in the Stroop tasks independent of trial type. By contrast, we found no modulation of Stroop interference effects or Stroop sequence effects. No inhibitory effects of cathodal stimulation were observed. These results support the causal role of the left DLPFC in working memory but lend no support to its involvement in Stroop interference control.