Since LED is a nonlinear semiconductor device, its linear model is difficult to establish and the corresponding controller cannot be designed using the linear system theory. To solve this problem, a constant-current Boost LED driver is taken as an example in this paper, and a control method of inverse-system decoupling control for double current loops is proposed. On the basis of the establishment of a large-signal averaged model of the system, a double-current loop control structure is adopted. Then, the inner and outer current loops are decoupled based on the inverse system theory, which are compensated as first-order integral subsystems, respectively. Moreover, the optimal control theory is adopted to design a controller for the linear subsystem. Simulation results show that the proposed control strategy can improve the steady-state and dynamic performances of the constant-current Boost LED driver. Finally, an experimental prototype was designed to further verify the correctness and effectiveness of the proposed control strategy from both the electrical and optical perspectives.