With growing concern over environmental sustainability and dwindling fossil resources, it is crucial to prioritise the development of alternative feedstocks to replace fossil resources. Spent coffee grounds (SCGs) are an environmental burden with an estimated six million tons being generated on a wet basis annually, globally. SCGs are rich in cellulose, lignin, protein, lipids, polyphenols and other bioactive compounds which are important raw materials for use in industries including pharmaceuticals and cosmetics. Furthermore, the energy sector has the potential to capitalize on the high calorific value of SCGs for biofuel and biogas production, offering a sustainable alternative to fossil fuels. SCGs are readily available, abundant, and cheap, however, SCGs are currently underutilized, and a significant amount are dumped into landfills. This review explores the potential of SCGs as a source of a value-added compound through various conversion technologies employed in the valorisation of SCGs into biochar, biofuel, and important chemical building blocks. The state-of-the-art, current knowledge, future research to stimulate the creation of sustainable products, and the challenges and economic feasibility of exploring SCGs in a biorefinery context are presented.