In order to better utilize the proteins in squid viscera (Dosidicus gigas), the effects of different pretreatments on the degree of hydrolysis (DH) and volatile compounds of hydrolysates were studied. The DH was used as an indicator to select alkaline protease as the optimal protease from 8 types of proteases. The hydrolysis conditions of alkaline protease and the flavor of the hydrolysates were investigated through single-factor, response surface methodology, and pretreatment-assisted hydrolysis experiments. The results showed that alkaline protease had the highest DH (42.08 ± 0.58%), with enzyme dosage of 1.5%, hydrolysis temperature of 45 °C, hydrolysis time of 5 h, and liquid-solid ratio of 4:1. The DH of the ultrasound group was significantly higher than other groups, with the highest DH (45.67 ± 0.34%) after ultrasound for 40 min (U40). The proportion of molecular weight < 1 kDa and the content of free amino acids (1613.64 mg/100 g) were the highest at U40. The electronic nose results indicated that the composition of organic sulfur and aliphatic compounds in U40 showed significant differences compared to other products. The U40 sample had the highest type and content of volatile compounds (especially benzaldehyde), which was more conducive to the volatilization of flavor substances. In conclusion, U40 pretreatment can effectively improve the DH and flavor of hydrolysates.