Diamond-like Carbon coatings are well-known for their excellent wear and friction reducing properties. Novel DLCs are constantly being developed that further these beneficial characteristics; this is often achieved by incorporating a dopant into the microstructure of the DLC. One dopant that is widely used currently in commercial settings, including F1 car engines, is silicon. Si doping can be, to some extent, regarded as a double-edged sword. This is because, whilst it has been reported as being able to reduce friction in certain environments, this usually comes at the cost of far higher wear than the corresponding un-doped DLC. The fundamental aspects of Si-DLC's friction and wear properties are explored herein with the goal of optimising the coating using fundamental tribochemical knowledge.