The development of practical and efficient methods for C-C and C-X bond formation has attracted a great deal of current attention with the advent of C-H functionalization reactions. Hydrocarbons are perhaps the most inexpensive and readily available materials, and utilisation of such materials for the synthesis of essential chemicals is virtually and economically pragmatic. The means to utilize easily accessible hydrocarbons not only represents a useful, potent and straightforward alternative, but also constitutes an excellent opportunity to improve our chemical knowledge about a relatively unexplored domain. Early examples using alkylarenes are generally limited to their conversion to aldehydes, carboxylic acids, and nitriles. This review intends to focus on the latest developments adopting modern strategies for sp(3) C-H functionalization of methylarenes to achieve a diverse range of important organic compounds.