Comprehensive design of alloy structure through a rational surface atomic arrangement, component, and well-defined shape will maximize atomic utilization and prompt fantastic oxygen reduction reaction enhancements. In this work, the Pt-Ni alloy hyperbranched nanostructures are synthesized successfully via a facile one-pot synthesis route without through any seeds or templates growth. The success of this approach relies on the use of cetyltrimethylammonium bromide (CTAB) to control the growth of branches on certain facets. The as-prepared Pt-Ni alloy hyperbranched nanostructures exhibit an enhanced catalytic activity toward oxygen reduction reaction in comparison with commercial Pt/C, owing to the synergistic effects among Pt and Ni atoms and the unique morphology of high branching degree. These findings provide a simple strategic design and a realizable method to create highly active catalysts for practical electrocatalytic applications. (C) 2018 Hydrogen Energy Publications LLC. Published by Elsevier Ltd. All rights reserved.