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The modifications of histological properties and chemical forces on heated surimi gels with starch addition (0–12 g/100 g surimi) were investigated. Two types of heating processes (direct heating and two-step heating) were carried out on surimi gels in order to reveal the effect of setting on mixed matrices. The results of transverse relaxation time showed less immobile water and free water converted into bound water in a matrix subjected to the setting process. Scanning electron microscope and light microscopy images revealed inefficient starch-swelling in two-step heated gels. Chemical interactions and forces in direct cooking gels were more vulnerable to starch addition, resulting in significant decreases in hydrophobic interaction and sulfhydryl content (p < 0.05). With the increment of starch, the disulfide stretching vibrations of the gauche–gauche–gauche conformation were reduced in both gel matrices. The structural variations of different components collectively resulted in changes in texture profile analysis and water holding capacity. Overall, the results demonstrated that starch addition had a great and positive effect on the weak gel matrix by direct heating.

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