The functionalized NiFe-LDH with photosensitized GQDs were synthesized through the hydrothermal route by differing the amount of GQDs solution and studied its efficacy towards the mineralization of textile dyes under visible light. The synthesized samples were characterized by XRD, FESEM, HRTEM, DRUV-Vis, RAMAN, XPS, and BET. The combined effect of the hexagonal carbon lattice in GQD and open layered porous structure of NiFe-LDH nanosheets results in the contraction of the lattice. Different reactive and conventional dyes were taken as representative dyes to evaluate the activity of the as-synthesized photocatalysts. The enhanced electron absorption/donor effect between GQDs and NiFe-LDH, and the growth of oxygen-bridged Ni/Fe-C moieties enable the composite to exhibit better photocatalytic activity. Both photocatalytic activity and characterization results confirmed that the GQD@NiFe-LDH nanocomposite heterostructure synthesized at 160 °C by taking 10 mL of GQDs aqueous solution named GNFLDH10 has a higher degree of crystallinity and has the best photocatalytic efficiency compared to other reported visible light catalysts. Specifically, the above optimized GQD@NiFe-LDH photocatalyst is capable of photo-mineralizing 50 ppm of Reactive Green in 20 min, Reactive Red in 20 min, and Congo Red in 25 min respectively following a direct Z-scheme mechanism with substantial reusability.