Experimental and theoretical studies of single-phase natural circulation flow and heat transfer under a rolling motion condition are performed. Experiments with and without rolling motions are conducted so the effects of rolling motion on natural circulation flow and heat transfer are obtained. The experimental results show the additional inertia caused by rolling motion easily causes the natural circulation flow to fluctuate. The average mass flow rate of natural circulation decreases with increases in rolling amplitude and frequency. Rolling motion enhances the heat transfer, and the heat transfer coefficient of natural circulation flow increases with the rolling amplitude and frequency. An empirical equation for the heat transfer coefficient under rolling motion is achieved, and a mathematical model is also developed to calculate the natural circulation flow under a rolling motion condition. The calculated results agree well with experimental data. Effects of the rolling motion on natural circulation flow are analyzed using the model. The increase in the flow resistance coefficient is the main reason why the natural circulation capacity decreases under a rolling motion condition.