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Summary: Poly-α-methylstyrene (PAMS), as an ideal mandrel material used in the fabrication of inertial confinement fusion (ICF) targets, its efficient degradation is the key to the quality of targets. However, there is a great challenge to achieve enhanced degradation. Here, we proposed the strategy to optimize the degradation of PAMS microspheres using di-tert-butyl peroxide (DTBP) as a degradation initiator. Experimentally, monodisperse PAMS microspheres with DTBP were controllably prepared by a microfluidic-based microencapsulation technique. Thermogravimetric results show that DTBP largely decreases the initial degradation temperature from 550 K to 450 K, which effectively promotes the thermal degradation of PAMS microspheres. Theoretically, DTBP can reduce the activation energy of degradation. Moreover, the potential energy surfaces were used to describe the degradation process at the atomic level. Our work brings a new direction for the study of mandrel degradation in ICF targets fabrication, and also provides a valuable reference for solving the pollution of waste plastics.