By combining the semiempirical density-functional based tight-binding optimization with density-functional theory single-point energy calculation at the PBE1PBE/6-311G* level, we propose an efficient computational approach to determine lowest-energy structures of large-sized carbon fullerenes. Our studies show that C-92 (D-3: 28) and C-94 (C-2: 43) are the new leading candidates for the lowest-energy structures of C-92 and C-94. Moreover, for the first time, the lowest-energy structures of C-98-C-110 are identified on the basis of the density-functional theory calculation. The lowest-energy isomers C-102 (C-1: 603) and C-108 (D-2: 1771) are readily isolated experimentally because they are much lower in energy than their other low-lying IPR isomers.