Continuous bead-free C-type cubic gadolinium oxide (Gd2O3) nanofibers 20-30 mu m long and 40-100 nm in diameter were sintered by sol-gel calcination assisted electrospinning technique. Dipole-dipole interaction of neighboring Gd3+ ions in nanofibers with large length-to-diameter aspect ratio results in some kind of superparamagnetic behavior: fibers are magnetized twice stronger than Gd2O3 powder. Being compared with commercial Gd-DTPA/Magnevist (R), Gd2O3 diethyleneglycol-coated (Gd2O3-DEG) fibers show high 1/T-1 and 1/T-2 proton relaxivities. Intense room temperature photoluminescence, high NMR relaxivity and high neutron scattering cross-section of Gd-157 nucleus promise to integrate Gd2O3 fibers for multimodal bioimaging and neutron capture therapy. (C) 2015 Author(s). All article content, except where otherwise noted, is licensed under a Creative Commons Attribution 3.0 Unported License.