The concept of mental toughness is widely used, but empirical evidence is required to fully understand this construct and its related variables. The purpose of this paper was to explore the relationship between: (a) mental toughness and coping, (b) mental toughness and optimism, and (c) coping and optimism. Participants were 677 athletes (male 454; female 223) aged between 15 and 58 years (M age = 22.66 years, SD = 7.20). Mental toughness correlated significantly with 8 of the 10 coping subscales and optimism. In particular, higher levels of mental toughness were associated with more problem or approach coping strategies (mental imagery, effort expenditure, thought control, and logical analysis) but less use of avoidance coping strategies (distancing, mental distraction, and resignation). Eight coping subscales were significantly correlated with optimism and pessimism. In conclusion, the relationships observed in this study emphasize the need for the inclusion of coping and optimism training in mental toughness interventions. © 2007 Elsevier Ltd. All rights reserved.