High offshore installation costs are a significant factor limiting the competitiveness of offshore wind energy. One efficient installation approach for floating offshore wind turbines is to preassemble the tower, nacelle, and rotor onshore and perform a single lifting operation to mate the superstructure with the floating foundation at the installation site. It is heavy lifting, due to the weighty payload. At the end of the mating process, a loadoff operation is conducted to transfer the preassembly to the floating foundation. It results in a sudden change in total force acting on the vessel and causes substantial acceleration and potential damage to the mechanism in the onboard nacelles. The magnitude of acceleration of the onboard nacelles can vary greatly at different release instants. In this research, a simplified two-degrees-of-freedom (DOF) (heave and pitch) model is also proposed to account for the heavy lifting process and variable ballast tanks. The sudden payload transfer is approximated using a hyperbolic tangent function to guarantee continuity and differentiability. The loadoff operation consists of the decision-making and vessel-stabilizing phases. Based on the nonlinear model predictive control method, a payload-transfer time selector and anti-pitch ballast controller have been developed to achieve optimal release time decisions and stabilize the vessel after payload release, respectively. Six-DOF simulation results show that the proposed algorithms are capable to a satisfying level of robustness of deciding the optimal payload release time instant, as well as limiting the peak and mean acceleration magnitudes of the onboard nacelles after payload release. The decision-making and control strategies may promote the sustainable energy transformation by extending the operation window and reduce the installation costs.