Porous organic polymers (POPs) possess versatile advantages, such as light weight, excellent stability, and high porosity. Hence, POPs could be ideal functional platforms. Herein, two multifunctional M-POPs were prepared via the Schiff-base reaction. They possessed good microporosity, remarkable stability, high-density N/O atoms, and excellent luminescence. Interestingly, the M-POPs achieved a good carbon dioxide-capture value of 17.1 wt% at 273 K and 1 bar, and provided excellent H2 capture of 1.0 wt% at 77 K and 1 bar. The M-POPs had many hydroxyl groups and nitrogen on the walls, which aided the formation of metal-coordination sites. The M-POPs had an excellent capacity for the detection of metal ions that was accurate, selective, and sensitive. Furthermore, phospholipid-coated M-POPs could be used to detect metal ions in living cells. These results provide a new design for multifunctional POPs. In this research, we synthesized multifunctional porous organic polymers as an ideal platform for gas uptake, metal ions sensing, and cell image.