To address the issues of low efficiency, high labor intensity, and susceptibility to damage during the manual harvesting of Volvariella volvacea, a mechanized harvesting device was developed to accommodate the growth characteristics of Volvariella volvacea. Thin-film sensors were used to measure the harvesting force values under both the bending method and the rotating method, incorporating two-finger and three-finger operation modes. The results indicated that the maximum force for the bending method was 4.60 N, while that for the twisting method was 2.91 N (peak values, n = 20 per method). The twisting method required less effort and posed a lower risk of damage. A four-suction-cup flexible end-effector was designed using silicone rubber material and equipped with a rotary cylinder. ANSYS 2022 R1 finite element simulation verified that under an applied force of 8 N, the surface stress on the Volvariella volvacea was less than 1.1489 MPa, meeting low-damage requirements. A Volvariella volvacea harvesting test rig was constructed, and performance tests were conducted. The results showed that the overall harvesting success rate was 96.65%, the damage rate was 2.03%, and the average time per harvest by the end-effector was 5.9 s. This study provides a theoretical foundation and technical support for the mechanized and intelligent harvesting of Volvariella volvacea, and is significant for promoting the high-quality development of the Volvariella volvacea industry.