The yield of squid has grown gradually; however, the lack of intensive processing has led to the slow development of the squid industry. In a previous study, some organic salts were found to improve the quality of squid surimi gel. Therefore, this research focused on the effects of sodium citrate (SC) and sodium tartrate (ST) on the quality of squid surimi gel. Physical measurements, such as gel texture, water-holding capacity, and color of squid surimi gel, were conducted. The addition of 2.5% SC and ST significantly improved the gel strength by 40.7, 57.0, 22.9, and 58.1%, respectively, of gel strength compared with the addition of: 1.5 SC, 3.5 SC, 1.5 ST, and 3.5% ST alone. Rheological measurements revealed that the addition of 2.5% SC or ST shortened the gel degradation temperature range (i.e., 2.5% SC or ST: 40-53°C; other treatments: 40-60°C) of the squid paste during heating. Results of chemical force analysis showed that the addition of a high quantity of salt accelerated protein aggregation and reduced hydrophobic interactions and disulfide bond formation. Finally, an increase in the number of β-sheets and a decrease in the bulk water content demonstrated that the addition of 2.5% organic salt could form squid gel with a better network structure. The findings provide a scientific basis for the development of high-quality squid surimi gel.