We synthesized Au-Cu bimetallic alloy films with a controlled mesoporous architecture through electrochemical deposition using an electrolyte solution containing spherical polymeric micelles. The composition of the alloy films can be easily controlled by tuning the ratio between the Au and Cu species present in the electrolyte solution. At low Cu content, cage-type mesopores are formed, reflecting the parent micellar template. Surprisingly, upon increasing the Cu content, the cage-type mesopores fuse to form vertically aligned one-dimensional mesochannels. The vertical alignment of these mesopores is favorable for enhanced mass and ion transfer within the channels due to low diffusion resistance. The atomic distribution of Au and Cu is uniform over the entire film and free of any phase segregation. The as-synthesized mesoporous Au-Cu films exhibit excellent performance as a nonenzymatic glucose sensor with high sensitivity and selectivity, and the current response is linear over a wide range of concentrations. This work identifies the properties responsible for the promising performance of such mesoporous alloy films for the clinical diagnosis of diabetes. This micelle-assisted electrodeposition approach has a high degree of flexibility and can be simply extended from monometallic compounds to a multimetallic system, enabling the fabrication of various mesoporous alloy films suitable for different applications.