The recovery of rare earth ions from industrial wastewater has aroused wide concern in recent years. In present work, we synthesized a novel three-dimensional adsorbent (denoted as LF-AA) by grafting loofah fiber with acrylic acid via ultraviolet radiation. The LF-AA was washed by boiling water and subjected to soxhlet extraction with acetone and then fully characterized by attenuated total reflectance Fourier transform infrared spectroscopy (ATR-FTIR) and scanning electron microscopy (SEM). Rare earth ion (Ce(III)) was selected as a model to validate its adsorption property. The saturation adsorption capacity for Ce(III) reaches 527.5 mg/g. Not only was this material highly efficient at adsorbing Ce(III) from aqueous solutions, it also proved to have ideal performance in regeneration; the total adsorption capacity of LF-AA for Ce(III) after six successive cycles decreased only 6.40% compared with the initial capacity of LF-AA. More importantly, the LF-AA can be easily separated from aqueous solutions because of its three-dimensional sponge natural structure. This study provides a new insight into the fabrication of biomass adsorbent and demonstrated that the LF-AA can be used as excellent adsorbent for the recovery of rare earth ions from wastewater.