Abstract: We successfully constructed TiO₂-pillared multilayer graphene nanocomposites (T-MLGs) via a facile method as follows: dodecanediamine pre-pillaring, ion exchange (Ti⁴⁺ pillaring), and interlayer in-situ formation of TiO₂ by hydrothermal method. TiO₂ nanoparticles were distributed uniformly on the graphene interlayer. The special structure combined the advantages of graphene and TiO₂ nanoparticles. As a result, T-MLGs with 64.3wt% TiO₂ showed the optimum photodegradation rate and adsorption capabilities toward ciprofloxacin. The photodegradation rate of T-MLGs with 64.3wt% TiO₂ was 78% under light-emitting diode light irradiation for 150 min. Meanwhile, the pseudo-first-order rate constant of T-MLGs with 64.3wt% TiO₂ was 3.89 times than that of pristine TiO₂. The composites also exhibited high stability and reusability after five consecutive photocatalytic tests. This work provides a facile method to synthesize semiconductor-pillared graphene nanocomposites by replacing TiO₂ nanoparticles with other nanoparticles and a feasible means for sustainable utilization of photocatalysts in wastewater control.