The processing of composite granules of waste coffee dust and hollow polymer microspheres with sucrose solution as binder with high-shear granulation is demonstrated as a precursor for subsequent conversion to highly porous, hierarchically porous, mechanically stable structured granules for CO2 capture. The optimization of the granulation parameters, such as binder volume, waste coffee dust to hollow polymer microsphere weight ratio, and the agitator & chopper speed of the granulator, produced near-spherical granules of 4–16 mm in diameter. Subsequent pre-carbonization followed by activation using KOH as a chemical activator yielded activated carbon granules (ACGs) in the 3–5 mm size range. The ACGs exhibited hierarchical porosity with a high specific surface area (350–1573 m2 g-1), total pore volume (0.14–0.54 cm3 g-1), and significant microporosity (0.08–0.50 cm3 g-1). These textural properties enabled high CO₂ adsorption capacities of up to 4.3 mmol g-1 and 10 mmol g-1 at 1 bar and 10 bar, respectively, at 20 °C. The ACGs demonstrated a CO₂/N₂ selectivity in the range of 17.7 to 21.2 and a moderate isosteric heat of adsorption (18–43 kJ mol-1), indicating physisorption and efficient regeneration potential. These findings highlight the potential of structured ACGs as a sustainable, high-performance material with ease of processing for practical CO2 capture and gas separation applications, contributing to circular economy goals through waste valorization. This work demonstrates a scalable shaping route from spent coffee waste to mechanically robust, hierarchically porous granules without a separate palletization step, suitable for practical CO2 capture applications and also contributing to circular economy goals through waste valorization.