Nonlinear control is an important subject drawing much attention. When a nonlinear system undergoes route-to-chaos, its response is naturally bounded in the time-domain while in the meantime becoming unstably broadband in the frequency-domain. Control scheme facilitated either in the time- or frequency-domain alone is insufficient in controlling route-to-chaos, where the corresponding response deteriorates in the time and frequency domains simultaneously. It is necessary to facilitate nonlinear control in both the time and frequency domains without obscuring or misinterpreting the true dynamics. The objective of the dissertation is to formulate a novel nonlinear control theory that addresses the fundamental characteristics inherent of all nonlinear systems undergoing route-to-chaos, one that requires no linearization or closed-form solution so that the genuine underlying features of the system being considered are preserved. The theory developed herein is able to identify the dynamic state of the system in real-time and restrain time-varying spectrum from becoming broadband. Applications of the theory are demonstrated using several engineering examples including the control of a non-stationary Duffing oscillator, a 1-DOF time-delayed milling model, a 2-DOF micro-milling system, unsynchronized chaotic circuits, and a friction-excited vibrating disk. Not subject to all the mathematical constraint conditions and assumptions upon which common nonlinear control theories are based and derived, the novel theory has its philosophical basis established in the simultaneous time-frequency control, on-line system identification, and feedforward adaptive control. It adopts multi-rate control, hence enabling control over nonstationary, nonlinear response with increasing bandwidth ? a physical condition oftentimes fails the contemporary control theories. The applicability of the theory to complex multi-input-multi-output (MIMO) systems without resorting to mathematical manipulation and extensive computation is demonstrated through the multi-variable control of a micro-milling system. The research is of a broad impact on the control of a wide range of nonlinear and chaotic systems. The implications of the nonlinear time-frequency control theory in cutting, micro-machining, communication security, and the mitigation of friction-induced vibrations are both significant and immediate.