Cocoa bean shells (CBSs) are a byproduct of the chocolate production process, representing the external layer of the cocoa bean. CBSs exhibit many interesting chemical and nutritional characteristics resulting in a very rich content of dietary fiber (DF) and antioxidant compounds such as phenolic acids and flavan-3-ols. The DF fraction of CBSs is notably rich in soluble dietary fibers (SDFs), which may be associated with fermentability and prebiotic properties. The objective of this study was the valorization of CBSs through enzymatic treatments, thereby increasing the solubility of DF and potentially augmenting fermentability. CBSs were treated both raw and defatted. Three sets of carbohydrases were used in order to impact the dietary fiber profile. Cellulase, xylanase, pectinase and their combinations were used to perform enzymatic treatments. The application of cellulase, xylanase and a combination of both enzymes proved effective in achieving a high SDF destructuring of the insoluble dietary fiber (IDF) fraction in both defatted and raw CBSs. Notably, the SDF/IDF ratio was significantly elevated in the enzymatically hydrolyzed samples (1.13–1.33) compared to the untreated CBSs (0.33). Furthermore, the various treatments did not affect the antioxidant activity or the content of the main bioactive compounds. These results provide a foundation for new opportunities in the biovalorization of CBSs through green techniques for a range of potential industrial applications in the food and nutraceutical sectors.