Whiskers, having large length/diameter ratio, are fiber-shaped single crystals. The technical possibility of using calcium carbonate whiskers as papermaking filler to replace conventional powder-like calcium carbonate was investigated. The results showed that it may be feasible to use calcium carbonate whisker as papermaking filler. Compared with conventional precipitated calcium carbonate, calcium carbonate whisker had higher retention efficiency. The use of calcium carbonate whisker also favorably affected the strength properties of paper sheets. A model was proposed to suggest the mechanism for paper strength improvement. The whiskers filled in paper sheets could increase the friction between fibers, thus increasing bonding strength. Moreover, the strength properties of paper were further improved because calcium carbonate whiskers were partly embedded in pulp fiber walls.