A unique ionic liquid polymer (ILP)-assisted method is developed for preparation of PdPt nanoparticles (NPs) on carbon nanotubes (CNTs). Due to its intrinsic hydrophilicity and regularly arranged imidazolium cationic functional groups, ILP induces the growth of uniform PdPt NPs with an average size of 3.5 ± 0.5 nm on CNTs. The cyclic voltammetry and amperometric studies indicated that the resulting PdPt NP/ILP–CNT nanohybrids have larger electrochemical surface area, better electrocatalytic performance, and higher stability towards the formic acid oxidation compared to NPs supported on the pristine CNTs. The excellent electrocatalytic performance is mainly contributed to the smaller particle size and more uniform dispersion of PdPt NPs. These results imply that PdPt NP/ILP–CNT nanohybrids are promising electrocatalytic material for formic acid oxidation. This work may also explore a universal approach to fabricate superior framework of metal nanocrystalline on CNTs for broad applications in energy systems and sensing devices.