In this paper, we report a novel route to obtain LiVMoO6 nanocrystals using a soft mechanochemical synthesis method. Powder X-ray diffraction, infrared, and Raman data indicated the formation of a single-phase LiVMoO6 with brannerite-type structure after 60-min milling time. The average particles size of the obtained LiVMoO6, derived from transmission electron microscopy data is about 46 nm. From UV-Vis diffuse reflectance spectrum, the direct band gap value (2.77 eV) of the material was estimated. The electrochemical characterization of the LiVMoO6 obtained was performed for the first time by assembling an all-solid-state cell, employing LiVMoO6 as a cathode active material. Discharge-charge measurements for 10 cycles were performed in the potential range from 1.8 to 3.7 V under a current density of 0.1 mA cm(-2) at room temperature. The assembled all-solid-state Li-In/80Li(2)S center dot 20P(2)S(5) glass-ceramics/LiVMoO6 battery presents a sustainable reversible capacity of 35 mAh g(-1) and a coulombic efficiency close to 100 % after the second to the 10th cycles.