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A new member of the IV–V compounds, germanium–phosphorus (Ge–P) compounds, has been shown in experiment and theory to have a tunable bandgap (E_g), excellent chemical stability, strong in‐plane anisotropy, and wide‐range optical absorption, all indicating a promising future in electronic and optoelectronic applications. In this work, the application potential of Ge–P compounds as nonlinear optical (NLO) materials in ultrafast photonics is studied for the first time. The strong light–matter interaction, broad and tunable E_p, and broadband and strong optical response make GeP a likely NLO material for photonics, especially in infrared photonic devices. In addition, 2D GeP nanosheets are mixed with poly(vinylidene fluoride) (PVDF) to obtain a GeP@PVDF composite film, which further improves the stability of the GeP and, for the development of organic photonic devices, helps to slow its degradation. From Z …