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Engagement with nature, through both direct sensory exposure and a sense of connectedness, has been shown to have a positive effect on psychological health; although the mechanisms mediating these effects remain obscure. Spirituality, which has been posited within ecopsychology frameworks to be experienced in and through a sense of relationship with nature, may be one such mediating variable. The aim of the present study was to determine the extent to which engaging with nature, through both exposure and connectedness, influences psychological health, and the role of spirituality in this relationship. 132 females and 58 males with a mean age of 36.8 years (SD = 13.1 years) completed surveys comprising (1) the Nature Exposure Scale, (2) the Connectedness to Nature Scale, (3) the Mysticism Scale, and (4) the psychological health subscale of the WHOQOL-BREF. Nature exposure and connectedness to nature were positively associated with psychological wellbeing and greater reported spirituality. Furthermore, through the implementation of a hierarchical regression and mediation analysis, positive relationships between both nature exposure and connectedness to nature with psychological wellbeing, were significantly mediated by spirituality. It is concluded that spirituality can be an important aspect of one's experience of nature and, as a consequence, the positive effects derived from it.