Photocatalytic degradation of organic contaminants has been proven to be one of the greatest economical and efficient techniques to address environmental pollution problems. Multi-walled carbon nanotubes (MWCNTs)/g-C3N4 (GCN) nanocomposites (NCs) were synthesized by a hydrothermal process aided by ultrasound to produce active photocatalysts. The effective synthesis of GCN, MWCNTs, and MWCNTs/GCN NCs was confirmed by X-ray diffraction (XRD) patterns. The fabrication of GCN nanosheets (NSs), the nanotubular structure of MWCNTs, and a network of neuron-like structures for MWCNTs/GCN NCs were all revealed by structural and morphological characterization. The elemental mapping of NCs containing the suitable quantity of MWCNTs revealed a uniform distribution of the sample's component elements. When the optical properties of the fabricated nanomaterials were examined by employing UV–visible spectroscopy, the results revealed a blue shift (a shift of maximum absorption to the UV region), which suggests that the addition of MWCNTs increased the band-gap energy. The behaviour of e––h+ pair recombination was revealed by measuring the charge carrier movement and trapping efficiency using photoluminescence (PL) spectroscopy. Crystal violet (CV) dye was photocatalytically degraded using prepared NCs in the presence of sunlight, and the synergistic effects of GCN and MWCNTs were examined. With a degradation efficiency of 99.32 %, MWCNTs/GCN NCs demonstrated the best sunlight-irradiated photocatalytic activity for CV degradation. The degradation of CV was discovered to follow pseudo-first-order kinetics. Throughout five consecutive studies, the NCs demonstrated the highest levels of catalytic efficiency and recyclability, with 5 % reduced degrading activities. The trapping tests showed that the primary reactive species involved in the breakdown of CV were the •O2– and •OH radicals.