Graphdiyne (GDY), a newly emerging 2D carbon allotrope, has been widely explored in various fields owing to its outstanding electronic properties such as the intrinsic bandgap and high carrier mobility. Herein, GDY‐based photoelectrochemical‐type photodetection is realized by spin‐coating ultrathin GDY nanosheets onto flexible poly(ethylene terephthalate) (PET) substrates. The GDY‐based photodetectors (PDs) demonstrate excellent photo‐responsive behaviors with high photocurrent (Pph, 5.98 µA cm‐2), photoresponsivity (Rph, 1086.96 µA W‐1), detectivity (7.31 × 1010 Jones), and excellent long‐term stability (more than 1 month). More importantly, the PDs maintain an excellent Pph after 1000 cycles of bending (4.45 µA cm‐2) and twisting (3.85 µA cm‐2), thanks to the great flexibility of the GDY structure that is compatible with the flexible PET substrate. Density functional theory (DFT) calculations are adopted to explore the electronic characteristics of GDY, which provides evidence for the performance enhancement of GDY in alkaline electrolyte. In this way, the GDY‐based flexible PDs can enrich the fundamental study of GDY and pave the way for the exploration of GDY heterojunction‐based photodetection.