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Corrosion significantly affects the structural behavior of members in a connection (i.e., the thickness of steel plates, the preload force of bolts, and the friction factor of steel plates). Safety assessment of corroded steel frames (i.e., beam-to-column connection, beams, or columns) has been a major concern in engineering. In this work, an experiment of accelerated corrosion testing is carried out to obtain corroded specimens connected with high-strength bolts, and the preload force of high-strength bolts (PF-HSB) is monitored throughout the whole stage of the corrosion testing. Before the corrosion testing, the PF-HSB caused by the stress relaxation is also recorded. The PF-HSB decreases rapidly in the first five hours after the final screwing of bolts and it keeps stable after 100 h. The PF-HSB is seriously affected by corrosion, which decreases by 30.0% of the original preload force when the corrosion rate of steel plate reaches 3.5%. A finite element method for predicting the PF-HSB after corrosion is proposed. An estimation model for the PF-HSB considering the stress relaxation is established. A degradation model for predicting the PF-HSB after corrosion is also suggested, and is in good agreement with experimental data. The results of this research are of great significance for the safety assessment of in-service steel structures.