A portion of the lime mud formed during the causticizing process in the recovery process of kraft pulping should be purged from the calcium cycle as waste before it is fed to the lime kiln; this ensures that the quality of the pulp and pulping chemicals is maintained. The discharged greenish-gray lime mud, which is often disposed as an industrial waste, has been transformed herein into a high-quality papermaking filler via the hybrid calcium carbonate (HCC) and post-HCC (pHCC) technology. Initially, the lime mud was heat-treated and then ground to small-size particles. The ground lime mud was preflocculated with calcium oxide by ionic polymers, and carbon dioxide was injected to the flocs to produce lime mud HCC (LHCC). To produce lime mud pHCC (pLHCC), only the ground lime mud was preflocculated first, calcium oxide was added next, and finally, carbon dioxide was injected to the flocs. The resultant products, LHCC and pLHCC, gave brightness as high as that of the ground calcium carbonate (GCC) in paper while a little higher brightness for pLHCC than for LHCC. They also enabled to increase bulk, stiffness, and tensile strength. Application of the LHCC and pLHCC technology to the lime mud could save waste disposal expenses and produce better-quality paper.