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Nano-titania (n-TiO2), due to its unique photocatalytic and hydrophobic properties, can be used to prepare self-cleaning cement-based smart building materials. The n-TiO2 degrades organic and inorganic pollutants through its photocatalytic action and convert them into non-toxic byproducts, i.e., improves the air quality. In this review, aspects such as methodologies of n-TiO2 synthesis, approaches for n-TiO2 loading on cementitious materials, photocatalytic properties, self-cleaning mechanism, and application of n-TiO2 in cement-based