Quasi-2D perovskites have emerged as a promising candidate material for displays owing to their high photoluminescence quantum yields and low-cost solution synthesis. However, achieving pure red quasi-2D perovskite films with luminescence centered at 630 nm and a narrow emission band presents a critical challenge for high-definition displays. Herein, by incorporating 18-crown-6 as additives that simultaneously passivate defects and regulate phase distribution, full iodine-based quasi-2D perovskite films with a single red emission peak and spectral stability are designed. Additionally, through the introduction of an appropriate amount of chlorobenzene and enhancement of annealing temperature, resulting in a narrower phase distribution, the full width at half maximum (FWHM) of the emission peak is significantly reduced. After optimization of the process, we fabricated quasi-2D perovskite films with pure red emission, which exhibited a PL peak at 627.9 nm and a narrow FWHM of 45.1 nm. Based on these pure red perovskite films, diverse complex patterns such as fluorescent anti-counterfeiting labels are implemented for data storage and information encryption. This study provides an effective approach toward developing quasi-2D perovskites with high color purity for high-definition purposes.