This research evaluated the preservative properties of flour from the alga Gelidium sp., which is a waste substrate resulting from commercial phycocolloid extraction. Gelatin-based biofilms, which included two different concentrations of red alga flour, were developed and used as packaging systems during refrigerated storage (up to 9 days at 4 °C) of Atlantic mackerel (Scomber scombrus) muscle. In all batches tested, a progressive decrease in quality could be observed in the muscle of the fish as the storage time increased. Compared with the control fish, the Gelidium alga flour extract had an inhibitory effect (p < 0.05) on microbial activity (total aerobes, psychrotrophs, and proteolytic bacteria), lipid oxidation (peroxide, thiobarbituric acid, fluorescence and polyene indices), lipid hydrolysis (formation of free fatty acids) and pH increase in refrigerated mackerel muscle. In contrast, no significant effect (p > 0.05) was observed on trimethylamine formation, Enterobacteriaceae, or lipolytic bacteria counts. A preservative effect resulting from the incorporation of Gelidium alga flour into the gelatin-based biofilm was observed, indicating both quality and safety enhancement. In accordance with current global interest in the search for natural and waste sources, a novel and beneficial use of Gelidium flour for enhancing the quality of refrigerated fish has been proposed.