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Creating heterojunctions or composites by incorporating noble metals offers a remarkable means to modulate the electronic charge transfer and the nonlinear optical (NLO) properties in 2D transition metal dichalcogenides (TMDCs). The response of such 2D‐TMDC‐noble metal composites to femtosecond (fs) infrared (IR) and terahertz (THz) radiation, however, remains vastly unexplored. While the linear optical characteristics of a prototypical 2D‐TMDC, namely, MoSe2 nanosheets incorporated with noble metal (such as Au, Pt, and Ag) nanoparticles in the UV–Vis and the THz spectral range, the NLO characteristics are measured using a 70‐fs pulse at 800 nm excitation is investigated. The results demonstrate a clear reduction of band gap with the incorporation of noble metals in MoSe2, indicating an effective charge transfer mechanism at play. Notably, the MoSe2‐noble metal nanocomposites depicted a significant enhancement in the THz conductivities. In addition, a dramatic 4‐fold enhancement in the third‐order nonlinear coefficient and ≈2‐fold enhancement in the third‐order NLO susceptibility is achieved in MoSe2‐Ag nanocomposite. These results univocally suggest that the noble metal‐based composites with suitable charge transfer channels promote enhanced carrier mobilities and tunable electron transfer dynamics, making these hybrid materials promising candidates for optoelectronic applications both at IR and THz frequencies. [ABSTRACT FROM AUTHOR]