Natural products and supplements are widely and increasingly used by the aging population for mood and cognitive symptoms. Evidence suggests that some supplements may be effective at treating a range of mood and cognitive symptoms. There is growing use of complementary and alternative medicine in the treatment of mental disorders because they may be seen as “safer” than traditional drugs, and because patients with mental disorders frequently use complementary and alternative medicine. We review the existing limited evidence of the efficacy and safety of natural products and supplements that are being used for treatment of mental disorders. More rigorous studies in the area of holistic and integrative treatment and preventive approaches for late-life mood and cognitive disorders are urgently needed.