Structural vibration control is used to ensure the safety of structures in service and has become an active research area in the past few years. In this study, uncertainties in structural dynamics are considered to propose an interval linear quadratic regulator (LQR) method based on an interval Riccati equation. Multi-objective optimization with non-probabilistic dynamic reliability as a constraint is performed to design an optimal uncertain vibration control system. To alleviate the difficulty of quantifying the probabilistic uncertainty and accurately characterize uncertainty information for small samples, multi-source uncertainties are regarded as interval parameters. The bounds on these uncertainties are determined, and the deterministic and uncertain parts of an interval state-space equation for vibration control are then formulated using an expanded-order matrix and the interval analysis method. Next, the interval perturbation method with a matrix series is used to develop a novel solution method for the linear inhomogeneous time-invariant equation in the interval state-space equation for the vibration control system and is used to accurately predict the interval bounds of the state responses. The conventional LQR method from modern control theory is used to propose a novel optimal control method based on a novel interval Riccati equation using the Lyapunov equation and interval uncertainty propagation. The proposed interval control method can be used to estimate the uncertain bounds of the controlled gain and cost function. A non-probabilistic dynamic reliability model is established to evaluate the reliability index of the system, which can overcome the limitations of the large computational cost of determining the probabilistic reliability. The deterministic controlled cost and uncertain states are considered as two optimization objectives with the proposed reliability constraint. The resulting constrained multi-objective optimal vibration control problem is designed and solved using c-DPEA. A flowchart is presented as a clear overview of the uncertain vibration control method, and the effectiveness of the proposed method is validated using two numerical examples. Different optimal control designs are obtained using different reliability constraints for quantitatively analyzing the safety of the control system.