This paper investigates the stability of horizontal nonlinear vibration of four-high cold mill under the effects of gyro-precession and eccentricity between rolls. The threshold value of chaos about Smale horseshoe commutation is given from Melnikov method, and the correctness of the result is verified by the fractal process of the attraction basin. Through the analyzes of bifurcation, maximum Lyapunov exponents and bi-parameter bifurcation, it is revealed for the effect of different parameters variation on the nonlinear dynamic behavior of horizontal vibration in rolling system. The results show, the fluctuation amplitude of horizontal force increases, the stable domain decreases, and once its value ≥3.5, it is necessary to prefer to the adjustment of parameter-exciting stiffness; meanwhile, it is noticeable that the critical points of damping and average force of the system with bifurcation or chaos appear hysteresis. The evolutions of system dynamics with four pairs of parameter changes confirm the quantitative optimal couple of one structural plus one process parameter in the system. Based on this, we can also find a balance between the average horizontal force and eccentricity, so as to optimize the structural design so that there is a proper and reliable eccentricity between the rolls. The results provide a theoretical reference for service stability and dynamic reliability of the rolling mill system.