Self-assembly of di-blcok copolymers (di-BCs) with precise control on morphologies and structures of nanomaterials makes it a promising technology for catalyst preparation. However, applications of the BC-synthesized Pt nanoparticles (NPs) on fuel cell have less been discussed. The major challenge may be the difficulty in achieving high-density nanopatterns which require a low degree of polymerization but a high effective segment-segment interaction parameter of the BC templates. As a resolution, sequentially double-or triple-layered BC route provides a new density-increased idea of harnessing these materials. In present work, monolayer of ordered and high-dispersed Pt-NP arrays with a density 27-folded has been achieved by the multiple di-BC routes consisted of identical self-assembly and plasma-cleaning processes. The multiplication has been proved to be equivalent to the duplication and oriented translation of the initial Pt-NP arrays, which provides not only a well-defined approach to control the spacing precisely, but also a bottom-up process to synthesize hexagonal-arranged arrays with predicable densities. Electrochemistry shows that the density multiplication has no negative effects on the Pt utilization of the monolayer arrays, and a remarkable ECSA value of similar to 114.5 m(2) g(-1) is found. Further characterization of the monolayer arrays as cathodic catalysts for PEMFC reveals that, neither the ohmic losses nor the mass-transport losses are enhanced after the density multiplication, and the power density of the PEMFC assembled here is significantly higher than that using commercial Pt/C catalysts. All the results demonstrate that the multiple di-BC approach has great potential in preparation of BC-synthesized Pt-NP arrays for fuel cell applications. (C) 2018 Elsevier Ltd. All rights reserved.