Two-stage harvesting is the main method used for the mechanized harvesting of peanuts in China, in which the pickup device is a core part of the combine harvester. In order to solve the problem of pod loss caused by “stack” and “loss picking” from peanut plants when using a traditional spring-finger cylinder pickup device, an optimal spring-finger cylinder peanut pickup mechanism was designed and its picking properties were tested. Based on the picking characteristics and picking force analysis when considering a peanut plant windrow, the ideal picking attitude and swing rule of the spring-finger were determined, and the cam slide, as the core element of the spring-finger cylinder peanut pickup device, was optimized. A mathematical model of the cam cylinder center line was established according to the swing law of the four picking stations utilizing the spring-finger. MATLAB and ADAMS were used to establish a simulation of the pickup mechanism, and kinematics and dynamics simulation analyses of the pickup mechanism were carried out. According to the design results, a prototype was constructed and a running pickup test was carried out. The peanut plant picking experiments indicated that the phenomenon of peanut plant stacking had significantly disappeared. Furthermore, through response surface analysis, the optimal working parameters of the picking device were obtained as follows: the forward speed Vm was 48.0 m/min, the rotational speed N was 50 r/min, and the ground height H was −16.8 mm. The picking rate of peanut plants was 99.21% and the pod loss rate was 1.79% under two harvesting conditions, with a peanut plant moisture content of 15% to 17%. This study provides technical support for the future design of picking devices for two-stage peanut pickup harvesters.