(copyright) 2022 by the authors. Licensee MDPI, Basel, Switzerland.Herein, we report the designing of a C3N4/BiOI heterostructure that is supported on gum acacia-crosslinked-poly(acrylamide) hydrogel to fabricate a novel nanocomposite hydrogel. The potential application of the obtained nanocomposite hydrogel to remediate crystal violet dye (CVD) in an aqueous solution was explored. The structural and functional analysis of the nanocomposite hydrogel was performed by FTIR (Fourier transform infrared spectroscopy), X-ray diffraction (XRD), transmission electron microscopy (TEM), and scanning electron microscopy (SEM). The different reaction parameters, such as CVD concentration, nanocomposite hydrogel dosage, and working pH, were optimized. The C3N4/BiOI heterostructure of the nanocomposite hydrogel depicts Z-scheme as the potential photocatalytic mechanism for the photodegradation of CVD. The degradation of CVD was also specified in terms of COD and HR-MS analysis was carried to demonstrate the major degradation pathways.