ABSTRACT The gelation and microstructural properties of the hybrid gel constructed by scallop (Patinopecten yessoensis) male gonad hydrolysates (SMGHs), κ-carrageenan (κ-C), and methyl-β-cyclodextrin (M-β-CD) were determined by utilizing rheometer, low-field nuclear magnetic resonance (LF-NMR), Fourier transform infrared spectroscopy (FTIR), as well as cryo-scanning electron microscopy (cryo-SEM). The rheological results of SMGHs/κ-C were improved by the addition of M-β-CD. The stronger synergistic effects between SMGHs and saccharides were also evidenced by the red shift in hydrogen bonds and blue shift in ester sulfate bonds of SMGHs/κ-C/M-β-CD and κ-C/M-β-CD. These situations jointly promoted the formation of a denser microstructure by cryo-SEM. SMGHs/κ-C/M-β-CD complex could promise a new strategy to develop functional hydrogels.