When harvesting Lycium barbarum L., excess amounts of detachments of the half-ripe fruit, unripe fruit, flowers, and leaves significantly affect the yield and adversely affect the subsequent processing, such as drying and grading. Finite element method (FEM) simulations and experiments of detachments were performed to harvest more ripe fruit and less half-ripe fruit, unripe fruit, flowers, and leaves. Three-dimensional (3D) models of the ripe fruit, half-ripe fruit, unripe fruit, flowers, leaves, fruit calyxes (flower calyx), fruit stems (flower stem), and branches were constructed using a 3D scanner, and material mechanics models of the above parts were established based on physical tests with universal testing machines. Detachment simulations and experiments of the ripe fruit, half-ripe fruit, unripe fruit, flowers, and leaves were performed to determine the detachment mechanisms and sequences. The detachment forces of each set of two parts were obtained. The field experiments showed that the detachment force between the fruit and calyx of ripe fruit was the lowest value of these forces, and only the ripe fruit was the first to detach from the calyx when harvesting. The results provided data support on the mechanics properties of wood and the optimization basis for the harvesting method of L. barbarum.