In this paper, bond degradation due to the desalination process of chloride-contaminated reinforced concrete is investigated. Four different constant voltages were applied to study the effect of the current on the desalination. Two constant current densities were applied for comparison. Two different electrolytes, NaOH and Ca(OH) 2, were used to examine the effect of electrolyte on the bond characteristics. Pullout specimens were cast and tested, using a single rebar pullout test. Three bond parameters of the bond strength, the critical debonding shear load per unit embedded rebar length and the shear stiffness per unit embedded rebar length were obtained to evaluate the bond quality after desalination. It is found that the bond characteristics decrease dramatically as the duration and/or the voltage of desalination increase. Using Ca(OH) 2 solution as the electrolyte, less bond loss is observed than using NaOH solution. A micro-hardness experiment shows that softening of concrete near the rebar becomes more apparent as the desalination duration and/or desalination voltage increase. A chemical titration experiment indicates that the accumulation of potassium and sodium ions increases as the desalination duration and/or desalination voltage increase. A pH value measurement shows that the desalination current increases the pH value of concrete near the rebar. More than two-thirds of chloride ions migrate out of the rebar–concrete interface in two weeks of desalination with desalination voltage greater than 10 V. Bond strength decreases approximately 40–60%.