Although pendulum tuned mass damper (PTMD) is one of the most classic and commonly used vibration control devices, it has clear limitation due to the natural feature of linear TMD. Additional stoppers for the pendulum string (PTMD-AS) were proposed and introduced to improve the PTMD's performance by triggering its nonlinearity. A 2-DOF model was established to analyze the dynamic response of the system subjected to harmonic excitation, and the governing equations were formulated using the Lagrange equation. The extended incremental harmonic balance (EIHB) method and the Runge-Kutta (R-K) method were utilized to calculate the frequency response and time history of the system. Nonlinear dynamic characteristics of the pendulum with stiffness hardening were explored in detail. Sensitivity analyses were performed to investigate the effect of stopper position. It was found that aperiodic responses or multiple solutions could be induced when the pendulum underwent significant stiffness hardening upon passing the additional stoppers. Finally, the effectiveness and robustness of PTMD-AS are demonstrated in a numerical simulation of a high-rise building subjected to random wind excitation based on wind tunnel experiments.