Tower fatigue and strength are crucial operational concerns of floating offshore wind turbines (FOWTs) due to the escalation of the vibration phenomena observed on these structures as compared to land-based ones. FOWT towers are excited by wave and wind polyperiodic disturbances yielding continual transient states of structural vibration that are challenging for vibration mitigation systems. Thus, the paper investigates a novel implementation of nonlinear optimal-based vibration control solutions for the full-scale, tension leg platform (TLP)-based, NREL 5MW wind turbine tower-nacelle model with a 10-ton tuned vibration absorber (TVA), equipped with a magnetorheological (MR) damper, located at the nacelle. The structure is subjected to excessive wave and wind excitations, considering floating platform motions derived from model experiments in a wave tank. The MR damper operates simultaneously with an electromagnetic force actuator (forming a hybrid TVA) or independently (a semiactive TVA). The study includes both actuators’ nonlinearities and dynamics, whereby the former are embedded in the Hamilton-principle-based nonlinear control solutions. The TVA is tuned either to the NREL 5MW tower-nacelle 1st bending mode frequency (TVA-TN) or to the TLP surge frequency (TVA-TLP). The optimal control task was redeveloped concerning the TVA stroke and transient vibration minimisation, including the implementation of the protected structure’s acceleration and relative displacement terms, as well as the nonzero velocity term in the quality index. The regarded model is embedded in a MATLAB/Simulink environment. On the basis of the obtained results, the TVA-TN solution is by far superior to the TVA-TLP one. All the regarded TVA-TN solutions provide a tower deflection safety factor of ca. 2, while reference systems without any vibration reduction solutions or with a passive TVA-TLP are at risk of tower structural failure as well as the hybrid TVA-TLP system. The obtained TVA stroke reductions of 25.7%/22.0% coincide with 3.6%/10.3% maximum tower deflection reductions for the semiactive/hybrid TVA-TN case (respectively) with regard to the previously developed approaches. Moreover, these reductions are obtained due to the sole control algorithm enhancement; thus, no additional resources are necessary, while this attainment is accompanied by a reduction in the required MR damper force. The lowest obtained TVA stroke amplitude of 1.66 m is guaranteed by the newly introduced semiactive control. Its hybrid equivalent ensures 8% lower primary structure deflection amplitude and reduced nacelle acceleration levels thanks to the utilisation of the force actuator of the relatively low power (ca. 6 kW); the trade-off is an increased TVA stroke amplitude of 2.19 m, which, however, is the lowest among all the tested hybrid solutions. The analysed reference passive TVA systems, along with a modified ground-hook hybrid solution, can hardly be implemented in the nacelle (especially along the demanding side–side direction). The latter, being the well-proven hybrid solution for steady-state tower deflection minimisation, yielded unsatisfactory results. The achievements of the study may be used for an effective design of a full-scale vibration reduction system for the TLP-based floating wind turbine structure.