Marine mussels secrete remarkable mussel adhesive proteins (MAPs) for adherence to the substrates upon which they reside. Inspired by the intermolecular cross-linking characteristics of MAPs, we report the synthesis of thermosensitive dopamine modified Pluronic copolymer (PluF127-Dopa) with high coupling efficiency. Under certain temperature and concentration, PluF127-Dopa copolymers in aqueous solution self-assemble into micelles and are able to rapidly form a more stable hydrogels upon addition of oxidizing reagents such as NaIO4, resulting from oxidative cross-linking of dopamine. UV-vis spectroscopy was utilized to identify the reaction intermediates. The sol-gel transition curves of cross-linked PluF127-Dopa hydrogels (CL-PluF127-Dopa) were determined by a vial inversion method. The critical gelation concentration of CL-PluF127-Dopa hydrogels was significantly lower than those for PluF127-Dopa and unmodified Pluronic F127. The apparent mechanical strength of CL-PluF127-Dopa hydrogels was dramatically enhanced compared to those unmodified Pluronic copolymer hydrogels, suitable for sustained drug delivery. These new biomimetic materials are expected to have potential uses in biomedical applications.