Single crystals of the new multiferroic Ba3NbFe3Si2O14have been synthesized and characterized via X-ray diffraction, magnetic susceptibility, NMR, and electric polarization measurements. The underlying topology of the Fe 3+spins is composed of isolated triangular units stacked in 2D layers along the c-direction of the trigonal lattice. Magnetic susceptibility experiments verify the spin state of the iron moments (S= 5/2), and large antiferromagnetic interactions with θ = −190 K. A cusp in the susceptibility and lambda-like feature in the specific heat indicate a magnetic phase transition at TN= 26 K, resulting in a frustration index of f= 7. A significant amount of spin entropy is released at higher temperatures, suggestive of short-ranged magnetic correlations developing at 50 K (as evidenced by features in the specific heat and thermal conductivity). The development of a spontaneous electric polarization below 26 K verifies that Ba3NbFe3Si2O14is a multiferroic. [ABSTRACT FROM AUTHOR]