Frozen molluscs (squid, octopuses, and cuttlefish) and crustaceans (shrimp) were irradiated using a cobalt-60 gamma source, at different doses, in order to investigate the effects of gamma radiation on their microbial population, organoleptic characteristics, lipid profile, and tropomyosin content. Irradiation of shrimp and squid with either 2.5 or 4.7 kGy reduced mesophilic bacteria contamination to low or nondetectable levels, respectively, whereas irradiation of octopus and cuttlefish with the same doses reduced the bacterial population. Irradiation treatment had no significant (P > 0.05) effect on the total lipid content and the major detected classes of polar and neutral lipids, whereas it significantly (P < 0.05) increased the contents of neutral lipids in octopus mantle and in shrimp muscle and cephalothorax samples. The total fatty acid content and the omega-3: omega-6 fatty acid ration was not affected. A dose-dependent significant (P < 0.05) decrease in the ratio of polyunsaturated fatty acids:saturated fatty acids was observed. With the increase in radiation dose, redness (a) and yellowness (b) values showed a variation, whereas the lightness (L) value was significantly (P < 0.05) decreased in mollusc mantles and shrimp muscle and increased in shrimp cephalothorax. The total of color changes ( delta E) increased (P < 0.05) as the dose increased. Significant (P < 0.05) changes in textural properties were observed with radiation treatment in octopus tentacles and in squid and cuttlefish mantle. The amount of tropomyosin, which is the major mollusc and crustacean allergen in the irradiated organisms, was reduced by gamma radiation, depending on the dose.