Background: Transcranial Direct Current Stimulation (tDCS) of the primary motor cortex (M1) can modulate neuronal activity, and improve performance of basic motor tasks. The possibility that tDCS could assist in rehabilitation (e.g., for paresis post-stroke) offers hope but the evidence base is incomplete, with some behavioural studies reporting no effect of tDCS on complex motor learning. Older adults who show age-related decline in movement and learning (skills which tDCS could potentially facilitate), are also under-represented within tDCS literature. To address these issues, we examined whether tDCS would improve motor sequence learning in healthy young and older adults. Methods: In Experiment One, young participants learned 32 aiming movements using their preferred (right) hand whilst receiving: (i) 30 min Anodal Stimulation of left M1; (ii) 30 min Cathodal Stimulation of right M1; or (iii) 30 min Sham. Experiment Two used a similar task, but with older adults receiving Anodal Stimulation or Sham. Results: Whilst motor learning occurred in all participants, tDCS did not improve the rate or accuracy of motor learning for either age group. Conclusion: Our results suggest that the effects of tDCS may be limited to motor performance with no clear beneficial effects for motor learning.