Shape- and size-controlled supported metal and intermetallic nanocrystallites are of increasing interest because of their catalytic and electrocatalytic properties. In particular, intermetallics PtX (X = Bi, Pb, Pd, Ru) are very attractive because of their high activity as fuel-cell anode catalysts for formic acid or methanol oxidation. These are normally synthesized using high-temperature techniques, but rigorous size control is very challenging. Even low-temperature techniques typically produce nanoparticles with dimensions much greater than the optimum <6 nm required for fuel cell catalysis. Here, we present a simple and robust, chemically controlled process for synthesizing size-controlled noble metal or bimetallic nanocrystallites embedded within the porous structure of ordered mesoporous carbon (OMC). By using surface-modified ordered mesoporous carbon to trap the metal precursors, nanocrystallites are formed with monodisperse sizes as low as 1.5 nm, which can be tuned up to ∼3.5 nm. To the best of our knowledge, 3-nm ordered mesoporous carbon-supported PtBi nanoparticles exhibit the highest mass activity for formic acid oxidation reported to date, and over double that of Pt-Au.