The sol-gel transition of methylcellulose (MC) solutions in the presence of ortho-methoxycinnamic acid (OMCA) or cetyltrimethylammonium bromide (CTAB) and in the coexistence of OMCA and CTAB was determined by the rheological measurement. It has been found that the sol-gel transition temperature of MC solutions increases linearly with the concentration of either OMCA or CTAB in solution, respectively. However, in the coexistence of OMCA and CTAB, the sol-gel transition temperature of MC solutions remains invariable, independent of the concentration of CTAB in solution. The experimental results show that OMCA has priority to adsorb on the methyl group of MC chains to form polymer-bound aggregates. In particular, these aggregates inhibit the hydrophobic interaction between CTAB and the methyl group of MC chains completely. Taking into account the fact that OMCA is almost insoluble in MC-free solutions but dissolves very well in aqueous MC solutions, we propose the formation of the core-shell architecture prompted by OMCA and the methyl group of MC chains, with the methyl group of MC chains serving as the core and the self-assembly of OMCA molecules serving as the shell. Obviously, the formation of the core-shell structure increases the solubility of OMCA, improves the stability of methyl groups of MC chains at high temperatures and inhibits the hydrophobic interaction between CTAB and the methyl group of MC chains in solution. The abnormal behavior relating to the sol-gel transition of MC solutions in the presence of OMCA or in the coexistence of OMCA and CTAB is therefore explained. Upon UV irradiation, the sol-gel transition temperature of MC solutions in the presence of OMCA, or in the coexistence of OMCA and CTAB, decreases notably. However, the dependence of the sol-gel transition temperature of MC solutions as a function of OMCA concentration, or CTAB concentration in the presence of OMCA, does not change after UV irradiation. The sol-gel transition of methylcellulose (MC) solutions in the presence of ortho-methoxycinnamic acid (OMCA) or cetyltrimethylammonium bromide (CTAB) and in the coexistence of OMCA and CTAB was determined by the rheological measurement. It has been found that the sol -gel transition temperature of MC solutions increases linearly with the concentration of either OMCA or CTAB in solution, respectively. However, in the coexistence of OMCA and CTAB, the sol-gel transition temperature of MC solutions remains invariable, independent of the concentration of CTAB in solution. The experimental results show that OMCA has priority to adsorb on the methyl group of MC chains to form polymer-bound aggregates. In particular, these aggregates inhibit the hydrophobic interaction between CTAB and the methyl group of MC chains completely. the fact that OMCA is almost insoluble in MC-free solutions but dissolves very well in aqueous MC solutions, we propose the formation of the core-sh ell architecture prompted by OMCA and the methyl group of MC chains, with the methyl group of MC chains serving as the core and the self-assembly of OMCA molecules serving as the shell. Obviously, the formation of the core-shell structure increases the solubility of OMCA, improves the stability of methyl groups of MC chains at high temperatures and inhibits the hydrophobic interaction between CTAB and the methyl group of MC chains in solution. The abnormal behavior relating to the sol-gel transition of MC solutions in the presence of OMCA Upon the UV irradiation, the sol-gel transition temperature of MC solutions in the presence of OMCA, or in the coexistence of OMCA and CTAB, reduces notably. However, the dependence of the sol -gel transition temperature of MC solutions as a function of OMCA concentration, or CTAB concentration in the presence of OMCA, does not change after UV irradiation.