Mental ill health is currently one of the leading causes of disease burden worldwide. A growing body of data has emerged supporting the role of diet, especially polyphenols, which have anxiolytic and antidepressant-like properties. The aim of the present study was to assess the effect of a high polyphenol diet (HPD) compared to a low polyphenol diet (LPD) on aspects of psychological well-being in the Polyphenol Intervention Trial (PPhIT). Ninety-nine mildly hypertensive participants aged 40-65 years were enrolled in a four-week LPD washout period and then randomised to either an LPD or an HPD for eight weeks. Both at baseline and the end of intervention, participants' lifestyle and psychological well-being were assessed. The participants in the HPD group reported a decrease in depressive symptoms, as assessed by the Beck Depression Inventory-II, and an improvement in physical component and mental health component scores as assessed with 36-Item Short Form Survey. No differences in anxiety, stress, self-esteem or body image perception were observed. In summary, the study findings suggest that the adoption of a polyphenol-rich diet could potentially lead to beneficial effects including a reduction in depressive symptoms and improvements in general mental health status and physical health in hypertensive participants.