Small angle neutron scattering (SANS) is used to compare nanostructured Sn-Co-C alloys produced by vertical axis mechanical attriting to those produced by magnetron sputter deposition. The attrited materials have grain sizes that vary with composition and are on the order of 60 angstrom in size. The sputter deposited materials are either amorphous or have a grain size of approximately 10 angstrom, depending on the composition. The SANS results are used to further understand the electrochemistry of these materials when used as negative electrodes for lithium-ion batteries and to understand why mechanically alloyed Sn-Co-C alloys are far from reaching their expected theoretical specific capacity while sputtered alloys achieve capacities much closer to the expected value. (C) 2009 The Electrochemical Society. [DOI: 10.1149/1.3239988] All rights reserved.