The Combined Axisymmetric Buoy (CAB), a vertical axisymmetric buoy, has the potential to deliver a high energy absorption power. Considering the CAB-Wave Energy Converters (WEC), in order to achieve higher efficiency, the Power Take Off (PTO) systems, which converts the float motion into energy output, needs to be properly controlled. In this paper, a PTO control method for a CAB-WEC under irregular wave conditions is proposed. Based on the semi-analytical solution obtained in the time domain, a numerical optimization is carried out. The optimal PTO damping coefficients under different wave conditions are obtained, by considering the parameter defined as “capture width ratio”. The expression of the optimal PTO damping coefficient in the frequency domain is derived by an analytical method. Based on the semi-analytical solution of time domain dynamic characteristics and analytical method, a comparison between frequency domain optimization and time domain optimization is presented. In general, the two approaches arrive to very similar conclusions, even if with the time domain methodology a slightly higher capture width ratio is achieved. The experimental results have been used to validate the time domain optimization method and the variation in optimal average capture width ratio results.