Integrated CO2 capture and conversion (ICCC) represents a key negative emission technology to achieve carbon neutrality, and the construction of dual function materials (DFMs) with high CO2 uptakes and catalytic activity is essential. In this work, cylindrical, spherical and flake Ni-CaO DFMs were synthesized by the extrusion, extrusion-spherization and squashing methods, respectively, and effect of granulation on the structure and ICCC performance of Ni-CaO DFMs was investigated. Results indicated that granulation adversely affected the CO2 bulk diffusion and adsorption since it would destroy the porous structures of DFMs. The Ni-CaO-P exhibited a high CO2 uptake of 14.28 mmol CO2/g in 650°C and 10%CO2, and a high CO yield of 5.63 mmol CO/g in reverse water-gas shift (RWGS) reaction in 5%H2. Compared to the powdered DFMs, CO2 adsorption capacities of the Ni-CaO DFMs pellets decreased significantly to 7.28~9.78 mmol CO2/g, while the catalytic conversion rate of CO2 has been significantly improved. Granulation played an important role in stabilizing the CO2 uptakes of the Ni-CaO DFMs pellets in multiple cycles. The Ni-CaO-P exhibited a high loss-in-capacity of 31.37% for CO2 capture within 12 cycles, while the loss-in-capacity of the DFMs pellets was lower (9.36~24.23%).