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Physical inactivity is a major global public health issue associated with a range of chronic disease outcomes. As such, the underlying motivation and barriers to whether or not an individual engages in physical activity is of critical public health importance. This study examines the National Heart Foundation of Australia Heart Week Survey conducted in March 2015. A total of 894 (40% female) Australian adults aged 25–54 years completed the survey, including items relating to motivation and barriers to being physically active. The most frequently selected responses regarding motivation for physical activity among those categorised as active (n = 696) were; to lose or maintain weight (36.6%, 95% CI 33.1–40.3), avoid or manage health condition (17.8%, 95% CI 15.1–20.8), and improve appearance (12.8%, 95% CI 10.5–15.5). Some gender differences were found with a greater proportion of females (43.8%, 95% CI 38.0–49.8) reporting lose or maintain weight as their main motivation for being physically active compared to males (31.9%, 95% CI 27.7–36.6). Among those categorised as inactive (n = 198), lack of time (50.0%, 95% CI 43.0–56.8) was the most frequently reported barrier to physical activity. While empirical studies seek to understand the correlates and determinants of physical activity, it is critical that beliefs and perceptions enabling and prohibiting engagement are identified in order to optimise physical activity promotion in the community.