To extend understanding of the bonding behavior of fiber reinforced polymer (FRP) and steel bars in self-compacting concrete (SCC), an experimental series consisting of 36 direct pull-out tests monitored by acoustic emission (AE) were performed in this paper. The test variables involved rebar type, bar diameter, embedded length, and polypropylene (PP) fiber volume content. For each test, the pull-out force and free end slip were continuously measured and compared with the corresponding AE signals. It was found that the proposed AE method was effective in detecting the debonding process between the FRP/steel bars and the hosting concrete. The AE signal strength exhibited a good correlation with the actual bond stress-slip relationship measured in each specimen. Based on the AE location technique, the invisible non-uniform distribution of bonding stress along the bar was further revealed, the initial location of damage and the debonding process were captured. Additionally, the contribution of bar-to-concrete load-bearing mechanism (chemical adhesion, friction, and mechanical interlocking) to sustain the pull-out force was effectively clarified by studying the collected signals in the frequency domain of AE methods. The experimental results demonstrate that the proposed AE method has potential to detect the debonding damage of FRP/steel bar reinforced SCC structures accurately.