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Questions hovering over the modulation of bandgap size and excitonic effect on nonlinear absorption in two-dimensional transition metal dichalcogenides (TMDCs) have restricted their application in micro/nano optical modulator, optical switching, and beam shaping devices. Here, degenerate two-photon absorption (TPA) in the near-infrared region was studied experimentally in mechanically exfoliated from single layer to multilayer. The layer-dependent TPA coefficients were significantly modulated by the detuning of the excitonic dark state ( ). The shift of the quasiparticle bandgap and the decreasing of exciton binding energy with layers were deduced, combined with the non-hydrogen model of excitons in TMDCs and the scaling rule of semiconductors. Our work clearly demonstrates the layer modulation of nonlinear absorption in TMDCs and provides support for layer-dependent nonlinear optical devices, such as optical limiters and optical switches.