The conceivable properties and potential applications of low-dimensional diamond(-like) structures, such as two-dimensional diamane and one-dimensional diamond tubes or fibres, are both diverse and exciting. However, a fundamental challenge remains: is it possible to realise diamond(-like) structures with dimensions approaching those of the diamond unit cell, over a large area, that is stable under ambient atmospheric conditions? This question relates to the intrinsic difficulty of synthesising low-dimensional diamond-like materials. In this talk, I will present our group’s experimental efforts toward addressing this challenge, focusing on the synthesis and application of fluorinated diamane (F-diamane). I will also share a few of our latest interesting discoveries related to the formation of low-dimensional diamond structures.