MoS2/CoAl-LDH/HCF was synthesized by biotemplated method. MoS2/CoAl-LDH/HCF had a 3D hierarchically porous morphology with high surface area. MoS2/CoAl-LDH/HCF hybrids showed excellent adsorption performance for CR. MoS2/CoAl-LDH/HCF showed better photocatalysis for CR degradation in visible light. MoS2/CoAl-LDH/HCF photocatalyst was stable and recyclable.