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Ultra-high-performance concrete (UHPC) has promising applications in civil engineering. However, the elastic modulus of UHPC is relatively low compared with its compressive strength, which may result in insufficient stiffness in service. This work was carried out to explore the feasibility of producing UHPC with high elastic modulus by nano-Al2O3 (NA). Based on particle densely packing theory, the initial mixture of UHPC was designed via the modified Andreasen and Andersen model. An experimental investigation was conducted to systematically examine the effects of NA on different properties of UHPC, including its fluidity, mechanical properties, durability, and microstructure. It was found that: (1) Compared with UHPC without NA, the flexural strength, compressive strength, and elastic modulus of UHPC were improved by 7.38–16.87%, 4.08–20.58%, and 2.89–14.08%, respectively, because of the incorporation of NA; (2) the addition of NA had a prohibiting impact on the threshold pore diameter and porosity of UHPC, which suggested that NA could be conducive to its pore structure; (3) the incorporation of NA led to a decline of 2.9–11.76% in the dry shrinkage of UHPC, which suggested that incorporating NA in a proper amount could reduce the risk of cracking and alleviate the dry shrinkage of UHPC; (4) the optimal amount of NA in UHPC was 1.0%, considering the effects of NA on workability, mechanical properties, microstructure, and the durability of UHPC. [ABSTRACT FROM AUTHOR]