In this paper, a model for Cr (VI) removal and optimization was made using a novel aerogel material, chitosan-resole CS/R aerogel, where a freeze-drying and final thermal treatment was employed to fabricate the aerogel. This processing ensures a network structure and stability for the CS, despite the non-uniform ice growth promoted by this process. Morphological analysis indicated a successful aerogel elaboration process., FTIR spectroscopy corroborated the aerogel precursor's identity and ascertained chemical bonding after adsorption. Owing to the variability of formulations, the adsorption capacity was modeled and optimized using computational techniques. The response surface methodology (RSM), based on the Box-Behnken design using three levels, was used to calculate the best control parameters for the CS/R aerogel: the concentration at %vol (50-90%), the initial concentration of Cr (VI) (25-100 mg/L), and adsorption time (0.3-4 h). Analysis of variance (ANOVA) and 3D graphs reveal that the CS/R aerogel concentration and adsorption time are the main parameters that influence the initial concentration of CS/R aerogel metal-ion uptake. The developed model successfully describes the process with a correlation coefficient of R2 = 0.96 for the RSM. The model obtained was optimized to find the best material design proposal for Cr (VI) removal. Numerical optimization was used and showed superior Cr (VI) removal (94.4%) under conditions of a CS/R aerogel concentration of 87/13 %vol, with an initial concentration of Cr (VI) of 31 mg/L, and an adsorption time of 3.02 h. These results suggest that the proposed computational model can obtain an effective and viable model for CS material processing and for optimization of the uptake of this metal.