Natural minerals are generally accepted as one of the most suitable carriers to support TiO2 in photocatalytic and other applications because of their abundance, low cost, large surface area, and easy recyclability. Hence, in this work, a novel OD/2D TiO2/kaolinite composite endowed with presence of oxygen vacancies and surface defect sites was synthesized through a mild sol-gel method combining with nitrogen induction. Ciprofloxacin (CIP) was taken as the main target organic pollutant to study the photocatalytic performance of the synthesized catalyst. The results showed that the nitrogen treated TiO2/kaolinite composite exhibited improving degradation performance for adsorption-photocatalytic elimination of CIP within broad radiation spectrum (200-800 nm). The synthesized composite exhibited enhanced reaction rate constant which is nearly 7.00, 2.54 and 3.13 times higher than that of bare TiO2 treated with air under UV, solar, and visible light, respectively. Moreover, the newly prepared composite also exhibited significant enhancement towards the removal of formaldehyde under both UV and visible light. Radical scavenger experiments and ESR results indicated that holes should be the main oxidizing species within broad spectrum in the degradation system. The enhanced activity of nitrogen treated composite is mainly attributed to the induced oxygen vacancies as well as the intimate interface contact between TiO2 and kaolinite, resulting in smaller grain size, higher light absorption ability, and faster carrier separation efficiency. It is expected that this high-efficiency composite photocatalyst based on natural minerals will be a promising candidate for the elimination of pharmaceutical and personal care products and volatile organic compounds within broad radiation spectrum.