A novel nonequilibrium approach combining low-temperature reactive sputtering and excimer laser annealing was developed to resolve the opposing requirements on crystallization and minimization of dopant loss for creating heavily nitrogen-doped TiO(2) (TiON) thin film. By retaining nitrogen dopant concentration in the sputtered film, the laser annealing allowed exploration of new material chemistry not generally available to the conventional approaches. Compared with the traditional thermal annealing, the excimer laser annealing created TiON thin film samples with a higher nitrogen dopant concentration, better crystallization, higher visible light absorbance, and faster degradation effect on organic pollutants. The crystallization process from excimer laser annealing was carried out at room temperature with minimal damage to the substrate, thus applicable to plastic/organic substrates. This approach could be easily applied to other dopant/thin film/substrate systems, opening up an unexplored avenue for creating thin films with novel properties for a broad range of potential technological applications.