Phosphorene, mono/few‐layered black phosphorous with advantages of tunable energy bandgaps and strong light–matter interaction, is fabricated by electrochemical intercalation with large area (≈3 µm) and controllable thickness (mainly four layers). Thanks to the direct gap and resonant absorption of four‐layer phosphorene at the telecommunication band, all‐optical thresholding and optical modulation are demonstrated for optical communications by using few‐layer phosphorene‐decorated microfibers. This device is experimentally verified as an efficient noise suppressor that can enhance the signal‐to‐noise ratio and reshape the deteriorated signal pulse, and also as an optical modulator that can switch the signal on/off by pumping light. The findings, as the first prototypic device of all‐optical thresholding and optical modulation, might facilitate the development of phosphorene‐based optical communication technologies.