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A facile method for the synthesis of 2,2‐disubstituted‐2H‐1‐benzopyrans from easily accessible tertiary propargylic alcohols and phenolic derivatives is described using a sulfonated tetraphenylethylene‐based hypercrosslinked polymer (THP‐SO₃H) as the heterogeneous organocatalyst. The organocatalyst can be easily recovered by filtration and reused up to five consecutive cycles with nominal loss in catalytic efficiency. The binding interaction of the synthesized benzopyrans with human serum albumin was investigated using fluorescence spectroscopy and molecular docking techniques.