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The non-Gaussian property and its influence on peak factors and extreme wind pressures on the long-span cylindrical roof are studied in this paper. Firstly, the moment-based Hermite polynomial model (HPM), which is used to determine peak factors of non-Gaussian processes, is briefly introduced. Then, wind tunnel tests for the scaled rigid roof model are carried out to measure wind pressures on the roof surface. The statistical and spatial distribution of non-Gaussian properties of wind pressure on the roof is demonstrated. Regions around curved edges along the span of the roof exhibiting strong non-Gaussian properties are found. Peak factors determined by the HPM are examined by wind tunnel results and then calculated for the entire roof. According to their distribution, the regions with considerable peak factors are found. Results indicate that the peak factor of constant 2.5 or peak factor following the Gaussian process assumption is far smaller than that determined by the HPM, leading to extreme wind pressures being underestimated by 40–50%. Hence, it is necessary to include the non-Gaussian properties of wind pressure when calculating their extreme values for such long-span cylindrical roofs.