CuS‐functionalized cellulose based aerogel (CBA) with 3D macroporous structure was synthesized by in situ deposition of visible light responsive CuS photocatalyst. Hexagonal CuS was deposited onto the outer and inner walls of CBA matrix. CuS/CBA composite catalyst has hierarchical porous structure and abundance in functional groups supporting CuS on CBA surface that enhance photodecomposition of methylene blue (MB). The CuS/CBA composite was characterized by XRD, FTIR, SEM‐EDS, Atomic Absorption Analysis, and XPS analysis. Photodegradation rate of MB by CuS/CBA composite catalyst in visible light was 94.1%, whereas, 67.4% for pure CuS. Initial MB concentration effects, pH change, and variations in CuS/CBA dosage on overall reaction kinetics were also studied. CuS/CBA composite catalyst carried out Photo‐Fenton like reactions which decomposed 97% MB within 6 min, by producing hydroxyl radicals from chemical and photocatalytic reactions. CuS/CBA composite catalyst was recycled and reused. It retained over 80% MB degradation rate even after five consecutive cycles. CuS/CBA composite can be used as biocatalyst for removal of organic dyes. © 2018 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2019, 136, 47404.