Investigating efficient and selective photocatalysts for water treatment can help address the energy crisis and numerous environmental issues associated with the use of current fossil fuels. As a shell, we used nickel-layered double hydroxide nanosheets on top of an anatase TiO2-carbon core to create an integrated photocatalyst. Materials were characterized using FTIR, XRD, SEM, HRTEM, and XPS methods for their physical-chemical properties. Using N2 adsorption/desorption at −196 °C, BET-surface area and pore structure were determined. Diffuse reflectance UV–vis was used to determine the photocatalysts band gap. For the TiO2-C/NiLDH amalgam, showed the lowest band gap (3.1 eV) with an exceptional ability to degrade methyl orange as an organic pollutant. Core–shell symmetry in the TiO2-C/NiLDH amalgam provides a larger surface area (72 m2/g) for interfacial interaction and a wider base for efficient charge transfer. In subsequent tests, this photocatalyst showed a remarkable level of stability and water treatment efficacy. That the TiO2-C/NiLDH amalgam can be used to alter solar energy and protect the environment has been demonstrated by these promising results.