We fabricated nanostructured Ge and GeSn films in He radio-frequency magnetron plasma sputtering deposition. Monodisperse amorphous Ge and GeSn nanoparticles of 30-40 nm in size were orderly arranged without aggregation by off-axis sputtering deposition in high He-gas-pressure range of 0.1 Torr. The Ge film porosity was over 30%. We tested the charge/discharge cycle performance of Li-ion batteries with nanostructured Ge and GeSn anodes. The Ge anode with an ordered arrangement of nanoparticles showed Li-storage capacity of 565 mAh/g after the 60th. The capacity retention was markedly improved by the addition of 3at% Sn in Ge anode. GeSn anode (3at% Sn) achieved a higher capacity of 1,128 mAh/g after 60th cycles with 92% capacity retention. Precise control of the nano-morphology and electrical characteristics by a single step procedure using low temperature plasma is effective for stable cycling of high-capacity Ge anodes.