Abstract: A type of novel organic-inorganic hybrid hydrogels were designed and synthesized by mixing the amino acids derived oligopeptides with 3-glycidoxypropyltrimethoxysilane (GPTMS). Considering the fact that the presence of closed cage POSS may result in unexpected swelling and biodegradability by silane condensation, hydrophilic carboxylized Pluronic was introduced to avoid the formation of POSS. Triethylamine (TEA) and carboxylized Pluronic were self-assembled into a supramolecular system with the aid of the intermolecular hydrogen bond and π-π stacking. Such a supramolecular system hindered the condensation polymerization of silane and disrupted the self-polymerization of GPTMS. The transversal and surface morphologies and chemical structure of the hybrid hydrogels were characterized by FTIR and SEM, their thermal degradability was characterized by TG, and their compression performance after aging for different time was measured by an electronic universal testing machine. The results indicated that the introduction of oligopeptides could hinder the self-condensation of GPTMS into the cage structure, and the epoxy groups of GPTMS reacted with the active hydrogen of TEA to form an organic network. The carboxylated Pluronic could help to form a supramolecular self-assembly system with TEA by the intermolecular force. Moreover, the self-assembled system exhibited a dependency of mechanical performance on the aging time, and it presented highest compressive strength of 8.6 MPa after aging for 24 h.