The rational design of semiconductor photocatalysts with multi-dimensional nanostructures is an effective way to solve the problem of water environmental pollution. Herein, a series of ZnIn2S4/MgAl-LDH (ZIS/LDH) composites with core-shell nanostructures were synthesized by in-situ growth of 2D ZnIn2S4 nanosheets onto the hexagonal LDH sheets. The obtained ZIS/LDH composite exhibited enhanced photocatalytic performance with 100% degradation efficiency for methyl orange (MO) within 20 min illumination, which was mainly attributed to the heterostructure formed by the excellent interface contact of the nanostructure, thereby inhibiting the recombination of photogenerated charges. Additionally, the as-synthesized photocatalyst shown satisfactory photocatalytic activity in stability tests and removal experiments for various dye pollutants. The present work provides a novel insight for the design of heterojunction photocatalysts with multidimensional nanostructures and environmentally friendly applications.