The dorsolateral prefrontal cortex (DLPFC) is part of a network important for emotional regulation and the possibility of modulating activity in this region with transcranial direct current stimulation (TDCS) to change mood has gained great interest, particularly for application in clinical populations. Whilst results in major depressive disorder have been promising, less is known about the effects of TDCS on mood in non-clinical populations. We hypothesized that multiple sessions of anodal TDCS applied over the left DLPFC would enhance mood, primarily as measured by the Profile of Mood States questionnaire, in healthy older adults. In addition, in an exploratory analysis, we examined the potentially moderating role of working memory training. Working memory, just like emotional regulation, taxes the DLPFC, which suggests that engaging in a working memory task whilst receiving TDCS may have a different effect on activity in this region and consequently mood. A total of 123 participants between 65 and 75 years of age were randomly assigned to receive either 20 sessions of TDCS, with or without working memory training, or 20 sessions sham stimulation, with or without working memory training. We found no support for enhancement of mood due to TDCS in healthy older adults, with or without cognitive training and conclude that the TDCS protocol used is unlikely to improve mood in non-depressed older individuals.