Veins and dikes of calcite-rich rocks within the Central Metasedimentary Belt boundary zone (CMBbz) in the Grenville Province of Ontario have been interpreted to be true carbonatites or to be pseudocarbonatites derived from interaction of pegmatite melts and regional Grenville marble. The putative carbonatites have been metamorphosed and consist mainly of calcite, biotite, and apatite with lesser amounts of clinopyroxene, magnetite, allanite, zircon, titanite, cerite, celestite, and barite. The rocks have high P and rare earth element (REE) contents, and calcite in carbonatite has elevated Sr, Fe, and Mn contents relative to Grenville Supergroup marble and marble mélange. Values of δ18OSMOW (9.9–13.3‰) and δ13CPDB (−4.8 to −1.9‰) for calcite are also distinct from those for marble and most marble mélange. Titanites extracted from clinopyroxene–calcite–scapolite skarns formed by metasomatic interaction of carbonatites and silicate lithologies yield U–Pb ages of 1085 to 1035 Ma. Zircon from one carbonatite body yields a U–Pb age of 1089 ± 5 Ma; zircon ages from two other bodies are 1170 ± 3 and 1143 ± 8 Ma, suggesting several carbonatite formation events or remobilization of carbonatite during deformation and metamorphism around 1080 Ma. Values of εNd(T) are 1.7–3.2 for carbonatites, −1.5–1.0 for REE-rich granite dikes intruding the CMBbz, and 1.6–1.7 for marble. The mineralogy and geochemical data are consistent with derivation of the carbonatites from a depleted mantle source. Mixing calculations indicate that interaction of REE-rich pegmatites with regional marbles cannot reproduce selected major and minor element abundances, REE contents, and O and Nd isotope compositions of the carbonatites.