Divalent calcium ions (Ca2+) are often used in surimi gels to improve their physicochemical characteristics. The present study aimed to investigate the effect of calcium lactate on the physicochemical properties, state distribution of water, and protein structure changes of surimi gels made from large yellow croaker. The results showed that the addition of calcium lactate (0%, 0.5%, 1.5%, 2.5%, 3.5%, and 4.5% on wet surimi) significantly (p < 0.05) increased gel strength and whiteness, while cooking loss decreased. The water-holding capacity increased first and then decreased. When calcium lactate was added to 1.5%, the water-holding capacity reached the best value. Using low-field nuclear magnetic resonance to study the distribution of water state, the bound water content first increased and then decreased with the addition of calcium lactate, reaching the highest at 1.5%. In addition, the relaxation time of immobilized water was shortest at the addition of 1.5% calcium lactate. Analyzing the protein structural changes by Raman spectroscopy showed that there was a significant decrease (p < 0.05) in the α-helix accompanied by an increase in β-sheets, turns, and random coils after the addition of calcium lactate. The above changes were due to the Ca2+ that was bound to the negatively charged myofibrils to form a protein-Ca2+-protein cross-linking. Therefore, the addition of calcium lactate had a significant positive effect on the gelling ability of surimi.