When peanuts are harvested, the high rate of pod crush and pods leakage are the main problems in the current peanut fruit picking process. Optimized peanut picking rollers help to improve peanut harvesting efficiency. This paper investigates the fruit picking system of a three-monopoly, six-row semi-feeding peanut combine harvester, in order to reduce the rate of crush and leakage of peanut pods during the picking process. Firstly, this article specifies the structure and basic parameters of peanut picking pairs of rollers. Secondly, this paper combines JKR (Johnson-Kendall-Roberts) model theory, crash model simulation analysis, a field test, and other methods. Motion and force analysis are presented in detail for the peanut picking mechanism and associated harvesting components. The optimum clamping chain speed, the angle of installation of the picking rollers to the clamping chain, and the picking rollers’ speed are determined. A three-factor, three-level regression orthogonal combination test was designed to obtain regression models for pod crushed and pods leakage rate. The regression model’s response surface analysis concluded that when the clamping chain speed is 0.84–1.2 m/s, the fruit picking roller angle is 10°–11.2° and the fruit picking roller speed is 442 r/min–500 r/min. It is the optimal working parameter for the three-monopoly six-row peanut combine harvester. At this point, the peanut harvesting requirements are met, and the overall performance is significantly improved. This paper lays the foundation for the development of the semi-feeding peanut picking system.