Enhancing cognitive functions through noninvasive brain stimulation is of enormous public interest, particularly for the aging population in whom processes such as working memory are known to decline. In a randomized double-blind crossover study, we investigated the acute behavioral and neural aftereffects of bifrontal and frontoparietal transcranial direct current stimulation (tDCS) combined with visual working memory (VWM) training on 25 highly educated older adults. Resting-state functional connectivity (rs-FC) analysis was performed prior to and after each stimulation session with a focus on the frontoparietal control network (FPCN). The bifrontal montage with anode over the left dorsolateral prefrontal cortex enhanced VWM accuracy as compared to the sham stimulation. With the rs-FC within the FPCN, we observed significant stimulationxtime interaction using bifrontal tDCS. We found no cognitive aftereffects of the frontoparietal tDCS compared to sham stimulation. Our study shows that a single bifrontal tDCS combined with cognitive training may enhance VWM performance and rs-FC within the relevant brain network even in highly educated older adults.