Granular activated carbons (GACs) were produced from sugarcane bagasse combined with one of two binders (corn syrup, coal tar) by physical activation and from pecan shells by physical and chemical activation. GACs were evaluated for their physical (hardness, bulk density), chemical (ash, pH), surface (surface area, pore size distribution, surface chemistry), and adsorption properties (molasses color removal, sugar decolorization) and compared with two commercial reference carbons. Results showed that larger surface area, a well-developed macro- and mesoporosity, and a minimal surface charge were desirable in GACs designed for sugar decolorization. Steam activation of pecan shells carbon was the only by-product-activation combination that produced GAC with all the above three desirable characteristics of a good sugar decolorizer. Chemical activation of pecan shells yielded GACs with high surface area and adequate pore size distribution but with large surface charge. In contrast, sugarcane bagasse-based GACs exhibited low surface areas and unsatisfactory physical/chemical properties.