In this paper, the complex control dynamics of a predator–prey Lotka–Volterra chaotic system are studied. The main purpose is to control the chaotic trajectories of two-predator one-prey system which was introduced by Samardzija and Greller (Bull Math Biol 50(5):465–491. https://doi.org/10.1007/BF02458847 , 1988). Lyapunov based nonlinear control and sliding mode control methods are used. The other purpose of this paper is to present the sliding mode control performances under different sliding surface choices. Based on the sliding mode control and Lyapunov stability theory, four alternative sliding surfaces are constructed to stabilize the chaotic two-predator one-prey model to its zero equilibrium point. The focused control signals realize the control from only one state which provides simplicity in implementation. Numerical simulations are demonstrated to validate the theoretical analyses and compare the effectiveness of proposed controllers for the chaotic Samardzija–Greller system.