We have successfully developed a facile, fast, and efficient synthetic methodology for direct fabrication of stable AuPt alloy nanostructure catalyst on Toray carbon (TC) as well as glassy carbon substrates without involving any additional stabilizer or surfactant through ultrasonic-waveassisted electrodeposition (USA-ED) using simple Au and Pt metal salt precursors in electrolyte solution. To know the real effect of ultrasonic waves on deposited particles, the same experimental methods also followed without ultrasonic waves. Size, morphology, surface composition, and surface structure of AuPt alloy nanostructures were investigated by field emission scanning electron microscopy (FE-SEM), energy-dispersive X-ray analysis (EDAX), X-ray diffraction (XRD), inductively coupled plasma mass spectrometry (ICP-MS), and cyclic voltammetric techniques. The observed results clearly reveal that the USA-ED method yields densely packed Pt-rich AuPt alloy nanostructure, which is a more active electrocatalyst for methanol oxidation, whereas the normal (i.e., without ultrasonic wave) ED method shows loosely packed homogeneous alloy AuPt nanostructure, which is very poor for methanol oxidation. More significantly, USA-ED of Pt-rich AuPt alloy nanostructured surface showed profound enhancement of both electrocatalytic activity and long-term stability of methanol oxidation when compared to ED of Pt nanoparticles, USA-ED of Pt nanoparticle surfaces, and also state-of-the-art commercial electrocatalysts with 30 wt % loading of Pt/C (E-TEK). These obtained results confirm that our synthetic methodology of USA-ED is effective for preparing Pt-rich AuPt alloy nanostructured electrocatalyst with excellent activity and stability in methanol oxidation reaction.