The synthesis and applications of composites based on layered double hydroxides (LDHs) and nanocarbons have recently seen great development. On the one hand, LDHs are versatile 2D compounds that present a plethora of applications, from medicine to energy conversion, environmental remediation, and heterogeneous catalysis. On the other, nanocarbons present unique physical and chemical properties owing to their low-dimensional structure and sp² hybridization of carbon atoms, which endows them with excellent charge carrier mobility, outstanding mechanical strength, and high thermal conductivity. Many reviews described the applications of LDH/nanocarbon composites in the areas of energy and photo- and electro-catalysis, but there is still scarce literature on their latest applications as heterogeneous catalysts in chemical synthesis and conversion, which is the object of this review. First, the properties of the LDHs and of the different types of carbon materials involved as building blocks of the composites are summarized. Then, the synthesis methods of the composites are described, emphasizing the parameters allowing their properties to be controlled. This highlights their great adaptability and easier implementation. Afterwards, the application of LDH/carbon composites as catalysts for C–C bond formation, higher alcohol synthesis (HAS), oxidation, and hydrogenation reactions is reported and discussed in depth.