There is an increasing global trend towards the uptake of Low-Carbohydrate, High-Fat (LCHF) diets. To date however, there is limited information about the food choice motivations, health perceptions and behaviours of LCHF dieters. This cross-sectional quantitative study explored differences between those on a self-reported “LCHF diet”, “other diet”, and “no diet”. Participants (N = 330: 43 males and 287 females), aged between 18 and 72 years (M = 39.66) completed an online survey that measured demographic and health characteristics, food choice motivations, health perceptions, and diet characteristics and food choices. The results showed that “LCHF diet”, “other diet” and “no diet” groups were not different in BMI or background health characteristics, but were significantly different in food choice motivations and health perceptions. Those in the “LCHF diet” group showed a stronger perception of wholegrains, sugars and refined wheat products, and vegetable oils as harmful to health compared to the “other diet” and “no diet” groups. In contrast, saturated fats were perceived to be beneficial to health significantly more by those in LCHF diet than the other two groups. Importantly, the differences in perceptions between groups were similar to differences in food choice motivations and food behaviours between groups. This research provides preliminary Australian data that characterises food choice motivations and health perceptions surrounding LCHF dietary patterns. The results of this study can be used to understand dietary behaviour and food choice patterns to better support practitioners, researchers and public health advocates in research and health promotion strategies.