nonlinear optics, [5] among others, because of their unique structures and excellent physical and optical properties. For example, with the saturable absorption (SA) effect, 2D layered nanomaterials like graphene, [6,7] graphene oxide, [8] topological insulators, [9,10] transition metal dichalcogenide, [11][12][13][14] black phosphorus, [15][16][17] and Mxenes [1][2][3][18][19][20] have been widely used for Q-switching and mode-locking laser pulses in solid-state or fiber laser systems. In addition, other nonlinear absorption and nonlinear scattering (NLS) responses of these nanomaterials have been used for optical limiting. [21][22][23] As a consequence, deep excavation and a systematic study of their nonlinear optical (NLO) properties are extremely important for the development of high-performance optoelectronic devices based on low-dimensional materials.Indium selenide (InSe) is a III-VI layered material that has become the focus of considerable interest because of its fascinating optoelectronic properties. [24][25][26] Given its high quantumsize confinement effect, InSe possesses a broad adjustable band gap from 1.25 to 2.6 eV when the bulk InSe is reduced to a few layers. [27,28] The variable band gap makes it suitable for use in optoelectronic devices, such as photodetectors [29,30] and photocatalysts. [31] Furthermore, InSe nanosheets have been studied in the NLO field; for example, reported by Hao, Huang, and Su et al. Reported the strong second-harmonic generation effect in InSe nanosheets; [32][33][34] Han and Xu et al. reported the SA response of InSe films excited by ns and ps pulses, and derived potential applications based on the excellent SA. [35,36] However, a systematic study on the NLO performance of InSe films under different pulse width scales is lacking. Therefore, it is necessary to evaluate the NLO response under different pulse widths, the results of which will serve as a foundation for further research and the exploration of potential applications of 2D materials.In this study, InSe nanosheets were synthesized using a liquid-phase exfoliation technique. UV-visible absorption spectroscopy, Raman spectroscopy, transmission electron microscopy (TEM), and field emission scanning electron microscopy (SEM) were performed to characterize the quality of the obtained nanosheets. The NLO response of the InSe nanosheets was investigated using the open-aperture Z-scan method under the excitation of both ns and fs pulsed light. The pump-probe method was utilized to monitor the optical modulation caused by SA and NLS competition under ns pulses. In addition, timeresolved pump-probe and transient absorption techniques were used to study the carrier relaxation process. This work reports the nonlinear optical properties and ultrafast carrier dynamics of indium selenide (InSe) nanosheets obtained via liquid-phase exfoliation under pulsed excitation with different durations. InSe nanosheets exhibit a better saturable absorption response under 6 ns pulse excitation than that under 380 fs excitation. In addit...