Chitosan-based cryogel particles were synthesized using the inverse Leidenfrost (iLF) effect, with glutaraldehyde employed as the cross-linker. The resulting cryogels exhibited a sponge-like morphology with micrometer-sized interconnected pores and demonstrated resilience, withstanding up to three compression-release cycles. These characteristics highlight the potential of chitosan cryogels for diverse applications, including adsorption and biomedical uses. We further investigated the influence of varying acetic acid concentrations on the properties of the chitosan cryogels. Our findings revealed that the particle size distribution of the cryogels ranged from 1300 to 2900 μm. As the concentration of acetic acid increased, the swelling degree of the chitosan cryogels decreased, stabilizing at an approximate value of around 6 at 0.03 mol of acetic acid. Additionally, the shift in the absorption peak of the OH and free amino groups from 3261 to 3404 cm−1 confirmed the cross-linking reaction between chitosan and glutaraldehyde.