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Considering the increase in research regarding environmental pollution reduction, the utilization of cementitious material, a commonly used construction material, in photocatalysts has become a desirable research field for the widespread application of photocatalytic degradation technology. Nano-reinforcement technology for cementitious materials has been extensively researched and developed. In this work, as a new and promising reinforcing agent for cementitious materials, the photocatalytic performance of titanium dioxide nanotube (TNT) was investigated. The degradation of methylene blue was used to evaluate the photocatalytic performance of the TNT-reinforced cement paste. In addition, cement paste containing micro-TiO2 (m-TiO2) and nano-TiO2 (n-TiO2) particles were used for comparison. Moreover, the effect of these TiO2-based photocatalytic materials on the cement hydration products was monitored via X-ray diffraction (XRD) and thermogravimetric analysis (TG). The results indicated that all the TiO2 based materials promoted the formation of hydration products. After 28 days of curing, the TNT-reinforced cement paste contained the maximum amount of hydration products (Ca(OH)2). Furthermore, the cement paste containing TNT exhibited better photocatalytic effects than that containing n-TiO2, but worse than that containing m-TiO2.