Reinforced concrete (RC) bridge columns are expected to undergo large inelastic displacements during major earthquake events, which in turn can result in residual displacements that can potentially affect the functionality of the bridge. While post-tensioning has been used to develop self-centering column systems for new bridge construction, the self-centering of existing bridge columns remains a challenge, mainly due to the limitations associated with the application of conventional post-tensioning techniques to existing structures. This study aims to address this important research gap by developing a robust self-centering technique to mitigate the residual displacements of the existing bridge columns. The proposed self-centering technique exploits the unique self-prestressing characteristics of iron-based shape memory alloy (Fe-SMA) bars to prestress existing bridge columns. The effectiveness of the proposed technique was evaluated through the large-scale experimental investigation of four columns. The variables of the study included the ratio of steel to Fe-SMA reinforcement, the total longitudinal reinforcement, and the initial prestress. The experimental results showed that the proposed technique could significantly reduce the residual drifts of existing bridge columns. The residual drift of the columns was found to be less than 1% up to a target drift of 4% when the ratio of steel to Fe-SMA reinforcement was ≤ 0.3. The paper concludes with a discussion of the self-centering mechanism of columns reinforced with prestressed Fe-SMA bars, where it is shown that, unlike post-tensioning tendons which do not contribute much to the energy dissipation of columns, prestressed Fe-SMA bars begin to contribute to the energy dissipation after the initial prestressing is lost at high drifts, resulting in an enhanced seismic resilience of the columns.