Methylcellulose and chitosan served as promising ingredients for a thermoresponsive hair styling gel after successful application in the medical industry. Both ingredients uphold the clean beauty standard without infringing on performance. By combining these two ingredients, a hair gel can be created that promises an extended hold of style once a heated external stimulus, such as a curling wand, is applied to the hair. Chitosan serves as the cationic biopolymer to adhere the gel to the hair, whereas the methylcellulose acts as the smart biopolymer to lock the desired hairstyle in place. Various ranges of chitosan and methylcellulose concentrations were explored for formulation optimization with rheology and curl drop testing. The rheology testing included a flow sweep test to understand the shear-thinning behavior of the sample as well as the effect of concentration on viscosity. Another rheology test completed was a temperature ramp test from room temperature (25 °C) to 60 °C to study the effect of heat on the various concentrations within the samples. A curl drop test was performed as well, over a 48-h period in which the different samples were applied to wet hair tresses, dried, curled, and hung vertically to see how the style held up over a long period of time with the influence of gravity.