The catalytic performance of noble metal nanocrystals highly depend on their surface structure and interface structure. The surface chemical functionalization of noble metal nanocrystals is a promising strategy for improving the catalytic/electrocatalytic activity, durability, and selectivity of the various important electrochemical reactions in low-temperature polymer electrolyte fuel cells. Herein, we demonstrate several approaches to synthesize a series of noble metal nanocrystals with chemical functionalization, including 0D nanodendrites, 1D nanowires, 2D platinum tripods with ultrathin and ultralong branches, and long-spined sea-urchin-like 3D nanostructures. Characterization results reveal that the organic polymeric amine strongly binds on the Pt surface. Loose-packed organic polymeric amine layers on the surface of nanostructures efficiently modify the electronic property of noble metal and serve as barrier networks to restrain accessibility of alcohol molecules. Due to the unique organic-inorganic hybrid concepts and structural features, the chemical functionalized noble metal nanocrystals show the high activity, excellent durability, and particular alcohol tolerance for the oxygen reduction reaction.