Spirulina (Artrhospira platensis) is rich in chlorophylls (CH) and is used as a potential natural additive in the food industry. In this study, the CH content was extracted from spirulina powder after ultrasound treatment. Microcapsules were then prepared at different ratios of gum Arabic (GA) and whey protein isolate (WPI) through freeze-drying to improve the chemical stability of CH. As a result, a* and C* values of the microcapsules prepared from GA:WPI ratios (3:7) were −8.94 ± 0.05 and 15.44 ± 0.08, respectively. The GA fraction increased from 1 to 9, and encapsulation efficiency (EE) of microcapsules also increased by 9.62%. Moreover, the absorption peaks of CH at 2927 and 1626 cm−1 in microcapsules emerged as a redshift detected by FT-IR. From SEM images, the morphology of microcapsules changed from broken glassy to irregular porous flake-like structures when the GA ratio increased. In addition, the coated microcapsules (GA:WPI = 3:7) showed the highest DPPH free radical scavenging activity (SADPPH) (56.38 ± 0.19) due to low moisture content and better chemical stability through thermogravimetric analysis (TGA). Conclusively, GA and WPI coacervates as the wall material may improve the stability of CH extracted from spirulina.