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Abstract: Here, the design and synthesis of a multispherical cavity carbon (MSCC) material with in situ silica modification and its application as anode catalyst supporter in proton exchange membrane fuel cells (PEMFC) are reported. The synthetic method involves a template procedure, where 10–30 nm sized silica nanospheres coated with polyvinylpyrrolidone (act as the substrate for aniline polymerization. Pyrolysis of the polymer layer and template etching lead to uniformly distributed MSCC materials. Both the pore sizes and the residue silica content in the inner cavities are controllable during the synthesis. It is further demonstrated that this MSCC material can be used as an anode catalyst supporter in PEMFC systems, where its self‐humidification properties result in enhanced durability. The MSCC‐supported anode exhibits only a 5.4% loss of current density and remains at 860 mA cm−2 after 10 h testing under nonhumidified condition, while commercial catalysts lost 25%. This justifies the promising application of MSCC in PEMFC systems. [ABSTRACT FROM AUTHOR]