Atime optimal sliding model controlwas proposed based on the fast acquisitionprocess of photoelectric tracking system. The sliding mode surface function of the control wasoptimal motion trail of time optimal control, which guaranteed that the system state variables slide along the optimal tracks; relevant exponential reaching lawwas designed to make the variables closer to sliding mode surface quickly and stably. Simulation and experiment research were carried out based on the capture targets of step signals of 180°, 90° and 60°.The experiment result shows that time optimal sliding model control and accommodation time decreases about 43.66% and 59.67% respectively compared with time optimal control and sliding model control. Besides, its overshoot and steady fluctuationare both 0, andsteady state errorsare decreased 44.94% and 62.34% approximately, whichare identical with the simulation result. The result indicates that the advantages of the method, such as short accommodation time, small overshoot, stable steady state value, little steady state error and strong robust, are applicable to quickly capture thephotoelectric tracking system and of significant research and application value.