Nylon 6 fabrics were chemically modified via reduction with BH 3 for being functionalized as heterogeneous base organocatalysts for Knoevenagel condensation. The results of FTIR, XPS, and SEM indicated the successful modification of nylon 6 fabrics. With a low catalytic dosage of 6.6 mol % and a short reaction time (2 h), the fabric catalysts were well applicable to Knoevenagel condensation of a wide range of substrates and up to 98% yield could be obtained. In addition, the fabric catalysts have some beneficial advantages in terms of easy separation, good reusability, and recyclability (up to 10 times).