Extracts that were obtained with solvents of increasing polarity (hexane, dichloromethane, methanol, 80% methanol, and water) from the red macroalga Gracilaria domingensis were evaluated by reducing power with ferric reduction antioxidant power (FRAP) and Folin–Ciocalteu (FC) assays, lipid peroxidation inhibition by β-carotene-linoleic acid assay, and metal chelating ability based on the iron-ferrozine system. The highest antioxidant capacity was reported for the hexane (Hx) extract by the FRAP, metal chelating, and lipid peroxidation inhibition assays. An activity-guided fractionation of the Hx extract was carried out for the identification of its active constituents. The primary components were the most active antioxidant compounds. Despite the high antioxidant activities, the Hx extract was not active in the FC assay. In this assay, the activities were found in the methanol (M) and 80% methanol (80M) extracts. The FC assay is commonly used to measure the total phenolic compounds. However, no phenolic compounds were detected by GC-MS and HPLC analyses in the M and 80M extracts. Thus, non-phenolic components influenced the FC assay. The M and 80M extracts showed high content of mycosporine-like amino acids (MAAs). A fraction contained two MAAs (porphyra-334 and shinorine) (156 mg GAE·g−1) showed a similar performance to the values that were found for well-known antioxidants (BHT = 156 mg GAE·g−1 and Trolox = 166 mg GAE·g−1) and 30 times higher than those of the original extracts (~5 mg GAE·g−1) in the FC assay. Thus, MAAs contribute to the antioxidant activities that were observed in the FC assay within the studied samples. Together, these results advance our understanding of the antioxidant properties of algal extracts.