To optimize the drying process of bamboo bundles, this study investigates the heat and mass transfer behavior during the drying process by using temperature sensors to measure the temperature field at different positions and track the overall moisture content over time. Additionally, a heat transfer model is used to simulate and predict the drying process. The analysis of the experimental results indicates that the diameter of the bamboo bundles has a greater impact on the drying rate than the drying temperature. At the same temperature, the drying time significantly decreases as the temperature increases. Under drying conditions at 80 °C, the average drying rate constant is 0.072 for bamboo bundles with a diameter of 40 mm, whereas it is only 0.015 for bundles with a diameter of 100 mm. Using Newton’s law of cooling, the convective heat transfer coefficient calculation method was derived. The average convective heat transfer coefficients at 40, 60, and 80 °C were calculated to be 6.16 W/(m2 K), 7.14 W/(m2 K), and 7.22 W/(m2 K), respectively. A mathematical model was established for the temperature at the center of the bamboo bundles, the temperature of the drying medium, the diameter of the bamboo bundles, and the drying time. This model effectively simulates the temperature variation inside the bamboo bundles, and the temperature simulation data fits well with the measured values, with a standard error of less than 2.8 °C and a prediction error of less than 6.1%. This coupled model and method provide a theoretical basis for predicting and controlling the bamboo bundle drying process, reducing energy and time consumption in actual production.