Due to the nonlinear, underactuated, and strongly coupled characteristics of tower cranes, issues such as inaccurate load positioning and severe swinging are prone to occur during transportation, making the control problem extremely complex. To address these issues, this paper has designed a super-twisting robust sliding mode controller based on the nonlinear marine predator algorithm (NMPA) to ensure the accurate positioning of the desired location during the transportation process of the tower crane while reducing the oscillation of the load. First, a nonlinear dynamic model of a four-degree-of-freedom tower crane considering friction is constructed. Second, to address the difficulty of effectively controlling the underactuated tower crane system model due to its nonlinearity and strong coupling, the super-twisting algorithm is introduced, and a super-twisting sliding mode controller for anti-swing positioning during the crane transportation process is designed. Then, the parameters of the super-twisting sliding mode controller are optimized using the NMPA to suppress sliding mode chattering and quickly achieve the system’s steady state. Finally, the stability of the nonlinear tower crane system is analyzed using Lyapunov’s theory and LaSalle’s invariance principle to ensure the closed-loop stability of the error dynamics. The simulation results show that the proposed control method exhibits excellent load anti-sway performance and robustness.