Previous works have found that the surface atomic structure and composition of catalysts play critical roles in the electrocatalytic performance of Pt-based catalysts. [5][6][7] Accordingly, nanoalloys with various atomic arrangement style including controlled composition or shape, core-shell structure, heterostructure, hollow structure and ordered structure have been designed and proved to be effective ways to modify the catalytic performance of Pt-based catalyst. [8][9][10][11][12] Furthermore, well-designed alloyed particles with Pt-enriched surfaces should possess a suitable electronic structure for ORR and thus meet both high performance and lower cost. [13] Low-coordination metal atoms often function as the catalytically active sites, while the specific activity per metal atom usually increases with decreasing size of the metal particles. [14,15] Additionally, smaller size also indicates higher dispersion of Pt atoms and higher utilization efficiency. [16] However, the surface free energy of metals increases significantly with decreasing particle size, promoting aggregation of small clusters. [17] Monodispersed superfine alloyed clusters have many advantages, such as high Pt-utilization efficiency and synergistic effects arising from neighboring metal atoms. [18] More importantly, by forming ordered intermetallic PtM nanocrystals with some metal M, the higher mixing enthalpy and stronger atomic interactions between Pt and M atoms would make PtM highly stable under electrochemical tests in both acidic and alkaline solutions. [19][20][21][22] However, in general, forming Industrial applications of Pt-based oxygen-reduction-reaction (ORR) catalysts are limited by high cost and low stability. Here, facile large-scale synthesis of sub-3-nm ordered Pt 3 In clusters on commercial carbon black as ORR catalyst that alleviates both these shortcomings is reported. As-prepared Pt 3 In/C exhibits a mass activity of 0.71 mA mg −1 and a specific area activity of 0.91 mA cm −2 at 0.9 V vs reversible hydrogen electrode, which are 4.1 and 2.7 times the corresponding values of commercial Pt/C catalysts. The asprepared ordered Pt 3 In/C catalyst is also remarkably stable with negligible activity and structural decay after 20 000 accelerated electrochemical durability cycles, due to its ordered structure. Density-functional-theory calculations demonstrate that ordered-Pt 3 In is more energetically favorable for ORR than the commercial Pt/C catalysts because ∆G O is closer to the peak of the volcano plot after ordered incorporation of indium atoms.