The effect of the maximum aggregate size and substitution rate of natural sand on the mechanical properties of concrete is evaluated using 15 lightweight aggregate concrete mixes. For mechanical properties of concrete, compressive strength increase with respect to age, tensile resistance, elastic modulus, rupture modulus, and stress-strain relationship were measured. The experimental data were compared with the design equations specified in ACI 318-08, EC2, and/or CEB-FIP code provisions and empirical equations proposed by Slate et al., Yang et al., and Wang et al. The test results showed that compressive strength of lightweight concrete decreased with increase in maximum aggregate size and amount of lightweight fine aggregates. The parameters to predict the compressive strength development could be empirically formulated as a function of specific gravity of coarse aggregates and substitution rate of natural sand. The measured rupture modulus and tensile strength of concrete were commonly less than the prediction values obtained from code provisions or empirical equations, which can be attributed to the tensile resistance of lightweight aggregate concrete being significantly affected by its density as well as compressive strength.