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As a rising star of all‐carbon nanomaterial, graphdiyne (GDY) has a direct natural bandgap and features strong light–matter interaction, large optical absorption, superior chemical and optical stability, indicating its broad prospects in the field of photonics and optoelectronics. Herein, the broadband nonlinear absorption and transient absorption characteristics of GDY from visible to infrared region has been studied for the first time, and its promising application in ultrafast photonics has been explored. The large nonlinear absorption coefficient (> −1 cm GW⁻¹), low saturation intensity (<13 GW cm⁻²), and ultrafast relaxation time (<30 ps) of GDY are demonstrated, which indicates the outstanding potential of GDY in photonics among the emerging novel nonlinear optical (NLO) materials. The GDY is mixed with polyvinylpyrrolidone (PVP) to prepare the GDY–PVP nanocomposite, which further improved the stability of …