The carbon aerogel (CA) uniformly doped neodymium oxide (Nd2O3) nanoparticle was synthesized by an effective in-situ method via acid catalyzing and used as the cathode matrix for lithium-sulfur batteries. The doped materials with interconnected pore structure of CA and evenly dispersed Nd2O3 offer crucial confinement role to anchor sulfur and suppress the loss of polysulfide ions for interrelate function of S/polysulfides by Nd2O3. The composited sulfur electrodes present high electrochemical performances and initial discharge capacities, especially, the Nd2-CA/S sample gains initial discharge capacity of 1327mAhg−1 at 0.2 C and remains at 1082mAhg−1 after 100cycles. Meanwhile, it still remains capacity of about 907mAhg−1 at 0.5 C after 300cycles. The enhanced electrochemical performances can be ascribed to the crosslink mesoporous CA materials and well distributed neodymium oxide. Furthermore, the metal additive also takes promoting effect on redox reactions of the Li/S batteries presenting higher discharge voltages.