UO2 kernels, a key component of fuel elements for high temperature gas cooled reactors, have usually been prepared by sol-gel methods. Sol-gel processes have a number of advantages, such as simple processes and facilities, and higher sphericity and density. In this study, to produce 900 μm-sized UO2 particles using an external gelation process, contact length extension of the NH3 gas of the broth droplets pass and the improvement of the gelation device capable of spraying 14 MNH4OH solution are used to form 3,000 μm-sized liquid droplets. To produce high-sphericity and high-density UO2 particles, HMTA, which promotes the gelation reaction in the uranium broth solution, is added to diffuse ammonium ions from the outside of the gelation solution during the aging process and generate ammonium ions from the inside of the ADU gel particles. Sufficient gelation inside of ADU gel particles is achieved, and the density of the UO2 spheres that undergo the subsequent treatment is 10.78 g/cm3; the sphericity is analyzed and found to be 0.948, indicating good experimental results.