A macaroni-like Li1.2V3O8 nanomaterial was directly prepared through a facile solution route using β-cyclodextrin (β-CD) as a template reagent. Its crystal structure was determined by the X-ray diffraction (XRD) pattern. From the scanning electron microscopy (SEM) and transmission electron microscopy (TEM) micrographs, we observed that the as-prepared Li1.2V3O8 material consisted of the aggregated macaroni-like nanoparticles and showed a porous structure. The electrochemical properties of the as-prepared Li1.2V3O8 in 1.0M Li2SO4 aqueous electrolyte were studied through cyclic voltammograms and charge–discharge measurements. The results revealed that the as-prepared Li1.2V3O8 could deliver the initial specific capacities of 189, 140, and 101mAhg−1 at 0.1, 0.5, and 1.0C, respectively. It suggests that the as-prepared Li1.2V3O8 should have an attractive future to be applied in aqueous rechargeable lithium battery (ARLB).