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Graphdiyne oxide (GDYO), the oxidized form of graphdiyne (GDY), has been widely explored for applica-tions in various technological fields owing to its fascinating properties. However, the research of GDYO for applications in photodetectors (PDs) and mode-locker has been lagging. Herein, we present experimental demonstrations of promising applications of GDYO for narrow-band photoelectrochemical (PEC)-type PDs with tunable performance. Moreover, the measured excellent nonlinear optical absorption of GDYO makes it a suitable material for mode-locking in ultrafast fiber lasers. Ultrastable pulses as short as 1.5 ps could be obtained from an Erbium-doped fiber laser based on GDYO at 1559 nm. These findings have been supported and interpreted by density functional theory (DFT) calculations as well as transient absorption dynamics studies. The presented results provide pathways for the future utilization of GDYO in high-performance optoelectronic devices.