To improve the pod-picking efficiency of the combine harvester for both peanut seedlings and peanuts, a longitudinal axial flow pod-picking device is designed in this study. The fixation and adjustment modes of the pod-picking rod were determined. The pod-picking roller’s rotational speed, the pod-picking roller’s diameter, the pod-picking roller, the pod-picking roller’s effective rod-picking length, and the screw-feeding stirrer’s critical parameters were determined by theoretical calculation. A combined design of quadratic regression orthogonal rotation was achieved by using Box-Behnken design (BBD) response surface optimization analysis in Design-Expert, with the linear speed of the pod-picking roller, the clearance between the concave screen and the pod-picking roller, and the spacing between the pod-picking rods as the testing factors, and the picking rate and the crushing rate as the indicators. The optimized parameters are as follows: a linear speed of the pod-picking roller of 6.8 m/s, a clearance between the concave screen and the pod-picking roller of 28.5 mm, and a spacing between the pod-picking rods of 18.60 mm. The performances of conventional peanut full-feeding pod-picking devices and the proposed peanut root-disk full-feeding longitudinal axial flow pod-picking device were investigated and compared to clarify the pod-picking performance of the proposed peanut root-disk full-feeding longitudinal axial flow pod-picking device under optimized parameters. The results showed that the picking and crushing rates of the proposed peanut root-disk full-feeding longitudinal axial flow pod-picking device under optimized parameters were 98.93 and 1.62%, respectively, both of which were superior to those of conventional peanut full-feeding pod-picking devices. A pod-picking device matching the combine harvester for peanut seedlings and peanuts was processed under optimized parameters. Field tests revealed that the picking and crushing rates of the proposed harvester were 99.07 and 1.58%, respectively, meeting the industry standards. These findings are instrumental in the further improvement of peanut pod-picking devices.