Configuring RE(2) O(3) nanocrystals with pseudo-2D morphologies confers substantive gains in relaxivities over equivalent spherical counterparts. The most promising arises from Gd(2) O(3) whose ionic transverse and longitudinal relaxivities were as high as r(1) = 12.7 mM(-1) s(-1) and r(2) = 17.2 mM(-1) s(-1) (dispersed in H(2) O, T = 37 °C & B(0) = 1.41 T), pointing to new opportunities to achieve high contrast MRI while concomitantly affording longer half-life potential in vivo.