Pyrene‐functionalized silicon hybrid porous polymer (TAPPy‐HPP) was successfully synthesized by Schiff base reaction using tetra(4‐aminophenyl)pyrene (TAPPy) and tetra(4‐formylphenyl)silane (TFS) as building blocks. This hybrid polymer was characterized using IR, solid‐state 13C and 29Si NMR, and elemental analysis. Its morphology was analyzed by PXRD and SEM. Thermal analysis using TGA shows that synthetic polymer has higher thermal stability than monomers at a temperature of 5% weight loss (Td5%) of 392 °C. Though TAPPy‐HPP has a Brunauer‐Emmet‐Teller surface area of 45.4 m2 g‐1, it adsorbed dyes with high efficiency, especially for the anionic dye Congo Red (CR) with an adsorption capacity of up to 358 mg g‐1. Moreover, TAPPy‐HPP showed excellent recycling and regenerative properties. This polymer is a promising candidate for a fluorescent chemical sensor for the absorption of dyes due to its exceptional physiochemical stability and intense luminescence.