There has been a significant amount of interest in tart cherries due to their health-promoting properties. However, full understanding about the limited bioavailability of polyphenols upon consumption is a critical challenge for the cherry industry. Also, much of the previous research catering to this problem has focused on sweet cherries and that leads to the knowledge gap in the area of tart cherry processing and nutrient bioaccessibility. The long-term goal of the study is to develop value-added tart cherry products with enhanced health benefits through particle size reduction (micronization) and microencapsulation to improve the extractability and bioaccessibility of polyphenol compounds. In our study, we conducted a comparative analysis of micronization methods for tart cherry pure and selected megatron and high-pressure homogenization (HPH), based on the desired particle size reduction obtained. With micronization, there was a significant increase in the polyphenol (including flavonoid and anthocyanin) extractability, perhaps due to the disruption of plant cell wall, which resulted in the release of metabolites into the extracellular environment. Furthermore, tart cherry pure was microencapsulated by spray drying with five combinations of two wall materials, maltodextrin (MD) and gum arabic (GA). The results showed a significantly higher release of polyphenols and flavonoids for microcapsules coated with MD: GA at 15%:15%. Upon storage at different temperatures (4C, 25C and 42C) and relative humidity conditions (11%, 22.5%, 32%, 57%, 75%) for 30 days, it was observed that an equal blend of MD and GA (15%: 15%) was the best wall material combination in improving the stability and the chemical properties of spray-dried tart cherry microcapsules. Also, upon sequential digestion in the mouth, stomach and intestine, it was found that there was an increase in the release of polyphenols up to 2 h (stomach) and then a sharp decline during the 4 h (intestine), possibly due to reduced stability of the flavylium cation at higher pH values. Our studies have thus demonstrated the importance of tart cherry pure processed with micronization and microencapsulation, to generate microparticles and spray dried microcapsules respectively, in improving the polyphenol extractability and bioaccessibility.