This study aimed to investigate the effects of glazing with sodium polyacrylate (SP) and D-sodium erythorbate (DSE) on the quality changes of squid during frozen storage. Frozen squid samples were randomly divided into seven groups: (1) CK (unglazed); (2) WG (distilled water-glazed);(3) SG (0.1% SP -glazed); (4) SG-1DSE (0.1% SP with 0.1% DSE -glazed); (5) SG-3DSE (0.1% SP with 0.3% DSE-glazed); (6) SG-5DSE (0.1% SP with 0.5% DSE-glazed); (7) WG-1DSE (0.1% DSE-glazed). The efficacy of the different coatings was evaluated using various indicators, such as water holding capacity (WHC), pH value, low field nuclear magnetic resonance (LF-NMR), color, malondialdehyde (MDA) content value, free amino acids (FAAs) content, intrinsic fluorescence intensity (IFI) and the total sulfhydryl content (SH) content. Intrinsic fluorescence intensity (IFI) and low field nuclear magnetic resonance (LF-NMR) were used as fast monitoring techniques to monitor changes in quality of squid samples. The results showed that compared with the CK and WG groups, coating with either SG or DSE alone resulted in reduced rate of moisture loss (p < 0.05), lipid oxidation (p < 0.05) protein degradation (p < 0.05) and prolonged its shelf-life. The combination of glazing treatment with SG and DSE (groups SG-1DSE, SG-3DSE and SG-5DSE) further improved the protective effects of coating, particularly in the SG-3DSE group. Therefore, the glazing of SG-3DSE is recommended to be used to control the quality of frozen squid and to prolong its shelf-life during frozen storage.