There is an urgent need to develop sustainable, renewable, and environment-friendly adsorbents to rectify heavy metals from water. In the current study, a green hybrid aerogel was prepared by immobilizing yeast on chitin nanofibers in the presence of a chitosan interacting substrate. A cryo-freezing technique was employed to construct a 3D honeycomb architecture comprising the hybrid aerogel with excellent reversible compressibility and abundant water transportation pathways for the accelerated diffusion of Cadmium(II) (Cd(II)) solution. This 3D hybrid aerogel structure offered copious binding sites to accelerate the Cd(II) adsorption. Moreover, the addition of yeast biomass amplified the adsorption capacity and reversible wet compression of hybrid aerogel. The monolayer chemisorption mechanism explored by Langmuir and pseudo-second-order kinetic exhibited a maximum adsorption capacity of 127.5 mg/g. The hybrid aerogel demonstrated higher compatibility for Cd(II) ions as compared to the other coexisted ions in wastewater and manifested a better regeneration potential following four consecutive sorption-desorption cycles. Complexation, electrostatic attraction, ion-exchange and pore entrapment were perhaps major mechanisms involved in the removal of Cd(II) revealed by XPS and FT-IR. This study unveiled a novel avenue for efficient green-synthesized hybrid aerogel that may be sustainably used as an excellent purifying agent for Cd(II) removal from wastewater.