Cocoa is among the most cultivated and important tropical crops in the world, and it is economically viable in the agro-pastoral systems of tropical Africa. Further, the amount of cocoa residue is steadily increasing due to the strong worldwide demand for chocolate products. This review of cocoa residue found that an average of 18 publications per year were published in the last 10 years. The most common type of publication on cocoa pod husks (CPH) was newspaper articles, which comprised 50% of the publications. This review examines the use of CHP in sustainable development, agrochemical materials, and agro-materials through their potential valorizations into high value-added products. Indeed, CPH is an abundant, accessible, and renewable resource of bioproducts, dietary fibers, nutraceuticals, functional foods, pectin, antioxidant compounds, theobromine, and minerals. Potential food applications of CPH include the production of flavor compounds, gums, texturing agents, and others. The production of biomaterials for food and non-food use, biofuels, and organic acids, such as lactic acid (the polymerization of which produces the PLA used in bioplastic production), are several potential areas for the biotechnological development of CPH and its fractions.