Neodymium-doped rare-earth oxycarbonates, Ln 2 O 2 CO 3 : x mol% Nd 3+ (Ln = La, Gd, and Y, 0 ≤ x ≤ 5), were synthesized by a simple flux method using a 0.476Li 2 CO 3-0.270Na 2 CO 3-0.254K 2 CO 3 eutectic mixture. The suitability of these oxycarbonates as stable, nontoxic bioimaging phosphors that exhibit near-infrared (NIR) emission under NIR excitation was investigated. Gd 2 O 2 CO 3 : x mol% Nd 3+ and Y 2 O 2 CO 3 : x mol% Nd 3+ were obtained in single-phase form with a hexagonal type-II structure. The particle sizes of the Gd 2 O 2 CO 3 : x mol% Nd 3+ and Y 2 O 2 CO 3 : x mol% Nd 3+ were on a submicron scale suitable for bioimaging, but that of La 2 O 2 CO 3 : x mol% Nd 3+ was outside the suitable range for bioimaging. Gd 2 O 2 CO 3 : x mol% Nd 3+ and Y 2 O 2 CO 3 : x mol% Nd 3+ showed characteristic emissions corresponding to the f-f transitions of Nd 3+. The strongest emission peak was observed at around 1064 nm under excitation at 823 nm in the samples containing 2 mol% of Nd 3+. The emission intensity of Gd 2 O 2 CO 3 : 2 mol% Nd 3+ was 1.25 times higher than that of Y 2 O 2 CO 3 : 2 mol% Nd 3+. The emission intensity of both phosphors was also significantly higher than that of the indocyanine green in practical use as a bio-imaging reagent.