In the global plan towards a sustainable energy future, proton exchange membrane fuel cell (PEMFC) technology enables high energy density, zero emission and efficient energy conversion and is therefore considered as a promising power source based on renewable energy. So far, this technology has not been commercialized to compete with conventional power sources, due to its low performance and high manufacturing cost. Electrocatalyst is one of the key materials determining the performance and cost of PEMFC as it is required for catalyzing the chemical reactions involved in fuel cell operation. Up to now, platinum is still the most widely used catalyst, and its high price and low stability hinder the final commercialization of PEMFC. This study develops a new catalyst based on Pt and Fe. The new catalyst has a fully ordered intermetallic structure and is entrapped within thin carbon layers. Experimental evidence shows that such a catalyst possesses a catalytic activity and durability much higher than conventional pure Pt catalyst. This finding is useful for reducing the Pt usage, improving the performance, and promoting the application of PEMFC. † Electronic Supplementary Information (ESI) available: Grain size distributions of PtFe/C, N 2 adsorption/desorption isotherms, XRD patterns for PtFe and PtFe 1.8 samples, TEM images of JM Pt/C catalyst, Potential cycling between 0.6 and 1.0 V, ORR polarization curves for different catalysts, CV curves and ECSA results, TEM images and particle sizes after ADT. See Catalytic activity and durability improvements are still the main challenges for fuel cell commercialization. To enhance nanocatalyst performance and durability for oxygen reduction reaction (ORR), we prepare 3.6 nm sized PtFe particles with a fully ordered intermetallic structure and entrap them in a porous carbon (PtFe@C). This nanocatalyst toward ORR exhibits 8-10 times enhancement in specific and mass activities over the commercial catalyst of Pt/C. Such a large enhancement is the highest, when compared with all other kinds of intermetallic catalysts reported in the literature.Accelerated durability testing has induced only a small change to the ordered structure and a minor loss of the activity after thousands of potential cycles under harsh electrochemical conditions. The high activity and durability are attributed to the fine-grained and ordered structure of the nanoparticle and the confining effect provided by the porous carbon. The nanoparticle, PtFe@C, represents a new strategy for performance optimization and cost reduction and promoting practical applications of fuel cells.