A simple chemical process for the direct synthesis of a nitrogen (N)-doped carbon aerogel (NCA) with highly dispersed Pt nanoparticles via a poly(ethyleneimine) (PEI)-assisted strategy is described. A resorcinol-formaldehyde (RF) gel was treated with water soluble cationic PEI, which mainly functions as an anchoring site for metal ions. The functionalized PEI chains on the surface of the RF gel resulted in the unique formation of chemical complexes, with PtCl62 anchored to the RF gel, and subsequent homogeneous metal nanoparticle growth. The abundant amino groups containing PEI grafted to the RF gel also allowed the nitrogen atoms to be incorporated into the carbon framework, which can directly be converted into a NCA. The spherical Pt nanoparticles in the resulting material (Pt/NCA) were highly dispersed on the surface of the NCA without any evidenced of agglomeration, even after a thermal annealing at 900 degrees C. Compared with a Pt/CA synthesized by a conventional reduction method, the Pt/NCA showed enhanced electrochemical performance with a high electrochemically active surface area (191.1 cm(2) g(-1)) and electrocatalytic activity (V-onset = 0.95 V vs. RHE) with respect to oxygen reduction. The superior electrocatalytic activities of the Pt/NCA can be attributed to the synergistic effect of the highly dispersed Pt nanoparticles and the N-doped carbon supports that were prepared using the PEI-assisted strategy. The findings reported herein suggest that the use of PEI can be effectively extended to broad applications that require the homogeneous deposition of metal nanoparticles. (C) 2016 Elsevier Ltd. All rights reserved.