A newly designed and fabricated novel nanocomposite composed of multiwalled carbon nanotubes (MWNTs), poly(benzimidazole) (PBI), and Pt nanoparticles. This composite is fabricated by the preparation of PBI-wrapped MWNTs (MWNT/PBI), followed by Pt loading onto the MWNT/PBI. As a result of the PBI wrapping, the loading efficiency of the Pt nanoparticles onto the MWNTs is dramatically improved up to 58.8% compared to that of the pristine MWNTs (41.0%). The process also allows homogeneous Pt immobilization onto the surface of MWNTs without any strong oxidation process for the MWNTs that is typically used for metal supporting on carbon nanotubes. Far-IR spectroscopy of the composite shows a peak from the PtN bonding, indicating that these improvements are derived from the coordination of the Pt ion with the PBI molecules. Cyclic voltammogram measurements reveal that the Pt nanoparticles deposited on the MWNT/PBI shows higher utilization efficiency (74%) for electrocatalysts compared to that on the pristine MWNT (39%).