Flexible and deformable calcium carbonate (FCC) with a high aspect ratio was developed by forming calcium carbonate on the surface of nanocellulose through an in situ calcium carbonate formation process. Nanocellulose from wood fiber became a linear core of the newly formed calcium carbonate to result in the flexible inorganic material. When used in papermaking, FCC can make the paper bulky due to its large size and strong due to the creation of less surface area of calcium carbonate. It can also make the surface smooth due to its deformability. The property of FCC depends on the quality of the nanocellulose, the nanocellulose-to-calcium carbonate ratio, and the processing conditions. FCC demonstrated its potential to be the main component of paper by occupying more than 50% of the papermaking raw materials. FCC may change the history of paper in that major component of the paper materials becomes limestone rather than wood fibers. This could lead to the protection of the forest, reduced production costs, and energy savings in the manufacture of paper materials.