Nanostructured rare-earth silicates are widely considered as environmental barrier coatings for the new generation of silicon-based composites. In current work, the nanostructured Lu2SiO5 coatings were deposited successfully using nanostructured Lu2SiO5 feedstocks by atmospheric plasma spraying (APS). Moreover, the nanomechanical properties of Lu2SiO5 coatings were characterized systematically by nano-indentation. Results indicate that the grain growth of Lu2SiO5 coatings is not obvious compared to Lu2SiO5 feedstocks. The nanostructured Lu2SiO5 coatings exhibit bi-modal nanomechanical properties. The elastic modulus and nanohardness of Lu2SiO5 coatings are 148.84 ± 28.00 GPa and 8.51 ± 4.12 GPa, respectively. In addition, the elastic work and plastic work of Lu2SiO5 coatings are 10.387 ± 1.283 nJ and 18.437 ± 6.823 nJ, respectively. The proportion of consumption of energy of Lu2SiO5 coatings is 0.636 ± 0.099 during indentation, which means that nanostructured Lu2SiO5 coatings process an excellent wear resistance.