In the application of nonlinear optical components, ideal nonlinear optical media typically need to possess high nonlinear absorption coefficients and large modulation depths, among other characteristics. The extreme thinness of two-dimensional (2D) materials, typically at the atomic scale, offers significant advantages in miniaturized optoelectronic devices. However, this also reduces the effective light-matter interaction length, ultimately limiting the achievable interaction intensity. To enhance their nonlinear optical response and unlock their full potential in nanophotonics, current research primarily focuses on two directions: one is to develop novel 2D quantum-confined material systems with enhanced intrinsic nonlinear optical responses; the other is to design effective performance modulation strategies based on nonlinear optical theory to enable precise regulation of nonlinear optical properties. Here, recent progress in tailoring third-order nonlinear optical responses of 2D materials is systematically reviewed here. Various strategies for modulating and enhancing third-order nonlinear optical responses in 2D materials are comprehensively discussed, which can be systematically classified into intrinsic regulation and light-matter interaction modulation. Moreover, the remaining challenges in modulating third-order nonlinear optical responses of 2D materials and perspectives on future research directions are discussed.