Deep eutectic solvents (DESs) are liquids formed from a mixture of salts and molecular species. DESs have remarkable solvent properties and are potentially "greener" alternatives to traditional volatile organic solvents for applications as diverse as electrochemistry and nanomaterial synthesis. The wide range of possible combinations of cations, anions and molecular species allow DES properties to be controlled for a particular application. This work will probe the nanostructure of a DES composed of a 1:1:2 molar ratio of ethylammonium bromide (EABr) to butylammonium bromide (BABr) to urea and compared with the 1:1 molar ratio DESs EABr:urea and BABr:urea to reveal the effect of cation alkyl chain length on nanostructure. Understanding DES nanostructure will aid in establishing structure-property relationships in DESs for facile tuning of properties for future applications.