Metadynamics is employed to sample the configurations available to calcium carbonate nanoparticles in water, and to map an approximate free energy as a function of crystalline order. These data are used to investigate the validity of bulk and ideal surface energies in predicting structure at the nanoscale. Results indicate that such predictions can determine the structure and morphology of particles as small as 3-4 nm in diameter. Comparisons are made to earlier results on 2 nm particles under constant volume conditions which support nanoconfinement as a mechanism for enhancing the stability of amorphous calcium carbonate. Our results indicate that crystalline calcitelike structure is thermodynamically preferred for nanoparticles as small as 2 nm in the absence of nanoconfinement.