Abstract: This paper reports a study on the reconstruction of broken Si-O-Si bonds in iron ore tailings (IOTs) in concrete. Limestone and IOTs were used to investigate the influence of different types of coarse aggregates on the compressive strengths of concrete samples. The differences in interfacial transition zones (ITZs) between aggregate and paste were analyzed by scanning electron microscopy (SEM) and energy-dispersive spectroscopy (EDS). Meanwhile, X-ray diffraction (XRD) and infrared spectroscopy (IR) were used to study microscopic changes in limestone and IOTs powders in a simple alkaline environment that simulated cement. The results show that the compressive strengths of IOTs concrete or paste are higher than those of limestone concrete or paste under identical conditions. The Ca/Si atom ratios in the ITZs of IOTs concrete samples are lower than those of limestone concrete; the diffraction peak of the calcium silicate phase at 2θ=29.5°, as well as the bands of Si-O bonds shifting to lower wavenumbers, indicates reconstruction of the broken Si-O-Si bonds on the surfaces of IOTs with Ca(OH)₂.