A modified sigmoid sliding mode control (MS-SMC) approach is proposed for stabilizing and tracking a quadrotor system with a nonlinear sliding surface, where the dynamics model is underactuated, highly coupled, and nonlinear. The constructed nonlinear sliding surface is based on the traditional sliding mode surface with a modified sigmoid function, allowing the initial value to quickly reach equilibrium. A new type of nonlinear SMC is applied for performance improvement of the quadrotor using the proposed modified sigmoid sliding surface. To control the quadrotor effectively, a double-loop control method is used to design the control rate, in which the position subsystem is the outer loop, and the attitude subsystem is the inner loop.With the Lyapunov function, the stability of the overall closed-loop system is ensured by stabilizing each subsystem step by step. Moreover, from a practical point of view, the system performance under the model uncertainties and external disturbances are also considered. The simulation results show that the proposed MS-SMC performs better than the conventional sliding mode control (CSMC) and the back-stepping sliding mode control (BS-SMC) in terms of stabilization and tracking against external disturbances.