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The objective of this study is to investigate the impacts of steam heat treatment parameters (e.g., temperature, time, and pressure) on the impact toughness of rattan (<i>Calamus simplicifolius</i>). The Box–Behnken design response surface analysis was employed to optimize the steam heat treatment parameters. Impact toughness was selected as the evaluation index, with single-factor tests conducted as a baseline for comparison. Changes in chemical composition, cellulose crystallinity, and pyrolysis properties were analyzed using X-ray diffraction (XRD), Fourier transform infrared (FTIR) spectra, Thermogravimetry–Fourier transform infrared (TG-FTIR) spectra, and wet-chemistry methods for both untreated control samples and the heat-treated samples. The results show that a 1 h steam heat treatment at 160 °C under 0.1 MPa pressure has the optimal process parameters for the rattan. The achieved impact toughness value closely matches the predicted value at 71.29 kJ/m². After the steam heat treatment, hemicellulose and cellulose contents decrease, whereas relative lignin content increases significantly, leading to improved toughness characteristics in <i>Calamus simplicifolius</i> samples. The TG results indicate that maximum weight loss occurs at temperatures of 352 °C, 354 °C, and 361 °C, respectively, for three different samples. This suggests that the thermal stability is enhanced as a result of the heat treatment. These findings will help optimize the heat treatments of the rattan material.