A personal construct psychology (PCP; Kelly, 1955/1991) framework was employed in an attempt to reveal a holistic understanding of mental toughness in the context of Australian Football. Eleven male coaches (M age = 42, SD = 9.62) with considerable playing and coaching experience at the elite level were interviewed using a PCP-based interview protocol. Transcribed verbatim data were analyzed using grounded theory procedures. Three independent categories (characteristics, situations, behaviors) were inductively derived and integrated into a model in which the importance of understanding each component individually was emphasized. The relationship between these three central categories was also highlighted. Results identified the key mental characteristics and their contrasts together with those situations that demand mental toughness, and the behaviors commonly displayed by mentally tough footballers. Conceptualized in the context of these three categories, mental toughness in Australian Football can be considered as a buffer against adversity but also as a collection of enabling factors that promote and maintain adaptation to other challenging situations. Practical implications of the findings are discussed and focus on issues pertaining to enhancing and/or developing mental toughness.