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Introduction Calcium silicate cements (CSCs) with the addition of nanohydroxyapatite and calcium carbonate play a critical role in dental applications. To further improve their properties, particularly radiopacity and biointeractivity, the fluoride-containing radiopacifier ytterbium trifluoride (YbF₃) was added to their composition, and biological and mechanical characteristics were evaluated. Methods YbF₃ was added to 3 different CSCs: cement I (CSC + calcium carbonate), cement II (CSC + nanohydroxyapatite), and Portland cement. Material characterization encompassed measurements of pH, calcium, ytterbium, and fluoride ion release; radiopacity; setting time; porosity; microindentation properties; wettability; and Fourier transform infrared spectroscopic, x-ray diffraction, and scanning electron microscopic analyses. Osteoblast- and osteoclast-like cells were grown on the materials' surface to evaluate their adherence. Results The addition of calcium carbonate, nanohydroxyapatite, and 30 wt% of YbF₃ improved radiopacity and the setting time of experimental cements. The pH values did not differ among the groups. The greatest ytterbium and fluoride releases occurred in the Portland cement + YbF₃ group. Combined x-ray diffraction and Fourier transform infrared spectroscopic analysis showed the presence of calcium hydroxide and calcium silicate hydrates. In addition, the presence of calcium ytterbium fluoride and ytterbium oxide proved that YbF₃ reacted with cement compounds. Wettability of cement I + YbF₃ was superior to other formulations, but its porosity and microindentation properties were weaker than in the Portland cement + YbF₃ mixture. Cement II + YbF₃ presented micromechanical indentation and porosity characteristics similar to the Portland-based cement formulation. Osteoclast- and osteoblast-like cells adhered to the cements' surfaces without alteration of the cell structural integrity. Conclusions YbF₃-containing CSCs with nanostructured hydroxyapatite and calcium carbonate are well suited for dental application. © 2015 American Association of Endodontists.