Porous ionic polymers (PIPs) hold significant promise as materials for water purification due to their high specific surface area, adjustable pore structures, and ionic pore channels. Nevertheless, the precise control and tuning of PIPs’ pore structures remain challenging, limiting their widespread application in water treatment. In this study, we present a novel approach for fabricating tunable porous pyridinium polymers based on porous pyrylium polymers. The pore structures and adsorption properties of these PIPs can be tailored by utilizing various primary amines as modifiers. The resulting PIPs exhibit exceptional removal efficiency for a variety of waterborne pollutants, including organic dyes, heavy metal ions, and pharmaceutical residues. Furthermore, these PIPs can be effortlessly regenerated and reused through simple washing steps. This work demonstrates a versatile and feasible method for developing novel PIPs for water purification, with potential applications in the field of environmental science.