To improve nitrogen (N) use efficiency and minimize environmental pollution caused by fertilizer overuse, novel bio-based large tablet controlled-release urea (LTCRU) was prepared using bio-based coating materials to coat large tablet urea (LTU) derived from urea prills (U). Nano fumed silica (NFS) was added to the bio-based coating materials to improve the slow-release properties. The surface area of the LTU and U was measured by three-dimensional scanning. In comparison to U, LTU had a smaller surface area/weight ratio, which can reduce the coating materials. Scanning electron microscopy analysis showed that the addition of NFS in bio-based coating materials reduced the porosity of the coating shells of LTCRUs and, thus, enhanced the N release longevity of the controlled-released fertilizer. Dependent upon the pores on the coating shells of LTCRU, two N release patterns were revealed. Because of the good release characteristics, the novel LTCRU shows great potential to support sustainable agricultural production. KEYWORDS: modified large tablet controlled-release urea, surface area, bio-based material, nano fumed silica, release rate