The hibiscus calyx contains 0.3–2.4% total anthocyanins, and is a promising source for naturally red food colorants. In this study, commercially available hibiscus calyces were subjected to ethanolic-aqueous extraction and chromatographic enrichment with the XAD-7HP resin, to create scalable, high-anthocyanin and low-acidity natural food colorants. Anthocyanins, organic and phenolic acids were monitored after each step using UHPLC-DAD and UHPLC-QQQ/MS. 75.67% total anthocyanins were recovered from calyces after double extractions, and the content increased by 8.50–14.90 times after the column enrichment, reaching 14.51–31.90% (by dry weight) in the final product. Chromatographic fractionation was also shown to effectively increase the total phenolic acids by 11.01–16.22 times, and remove an average of 98.58% of the total organic acids. High intensity redness at pH 2.5–3.5 indicated that the final product may be a promising, versatile natural food and beverage colorant in low pH products.