Oil peony is an important oil crop that is primarily sown by using artificial methods at present. Its seeder encounters the problems of low efficiency of seeding that significantly limits the highly efficient mechanized production of high-quality peony oil. In this study, Fengdan white oil peony seeds were used as the research object and repose angle as the response value to establish a discrete element model (DEM) and parameter calibration. The range of parameters of oil peony seeds was first obtained through an experiment, and their repose angle was obtained by an inclinometer. A three-dimensional DEM of oil peony seeds was then established. The Plackett–Burman (PB) test was utilized to screen the parameters that had a significant influence on the repose angle, and the steepest ascent (SA) test was applied to determine their optimum range of testing. Following this, based on Box–Behnken (BBD) test results, a second-order regression model between the important parameters and the repose angle was constructed. Finally, the absolute minimum difference between simulated and measured repose angles was utilized as the objective of optimization to obtain the following optimum combination of parameters: The values of the seed–steel collision recovery coefficient (CRC), seed–seed static friction coefficient (SFC), seed–steel SFC, and seed–seed rolling friction coefficient (RFC) were 0.704, 0.324, 0.335, and 0.045, respectively. This optimal combination of parameters was confirmed through simulations, and the error between simulated and measured repose angles was only 0.67%, indicating that the calibrated DEM of oil peony seeds was reliable.