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In this work, molecular dynamics simulation is used to study the effect of hygrothermal conditioning on carbon fiber/epoxy interface. By simulating the debonding process, it is measured that the interface possesses lowest adhesion in high-temperature saltwater, which is related with the epoxy mechanical degradation, as demonstrated by the depressed glass transition temperature. Meanwhile, the softened epoxy molecule in hygrothermal conditioning possesses decreased density and more severe energy concentration near the fiber surface, which inhabits the stress transfer between fiber and matrix and leads to the deteriorated interfacial adhesion. The research findings contribute to the nanoscale insight into interfacial deterioration mechanism of CFRP composites in hygrothermal environment.