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Traditional phosphoric acid (PA) doped polybenzimidazole (PBI) membranes encounter many issues when used in high-temperature proton exchange membrane fuel cell (HT-PEMFC), including the loss of PA within the membrane and limitations on conductivity. The mixed matrix membranes (MMMs) synergistically combine the advantages of pore fillers and polymer matrix, making them promising candidates for HT-PEMs. Interface compatibility is the main factor affecting the further development of MMMs. This research presented OPBI composite membranes filled with porous nanosheets, featuring average pore diameters of 2.83 nm, 3.38 nm, and 2.60 nm, respectively. The high aspect ratio and plentiful nitrogen components of the nanosheets increase the π-π and hydrogen bonding interactions with the polymer matrix, resulting in outstanding interface compatibility and mechanical properties of MMMs. The results of theoretical calculations indicate that there is a stronger interaction energy between the nanosheets and PA molecules, and the abundant pore structure within the nanosheets facilitates the absorption of PA molecules, leading to the formation of a continuous PA network. Consequently, MMMs exhibited enhanced proton conductivity, as well as improved PA absorption and retention. Furthermore, the effect of pore size distribution of nanofillers on the performance of MMMs were investigated. Membranes composed of nanosheets with large pore size showed a higher conductivity of 176.7 mS cm−1 at 200 °C, leading to excellent performance and stability in assembled H 2 /O 2 fuel cells. This work offers valuable insights into the design of MMMs and high-performance HT-PEMs. [Display omitted] • Porous nanosheets have high aspect ratio and rich nitrogen content. • Porous nanosheets have excellent interface compatibility with polymer matrices. • Mixed matrix membranes have higher PA absorption and retention compared to OPBI membrane. • Faster proton transport networks can be formed with the use of large pore size nanosheets. [ABSTRACT FROM AUTHOR]