The effective utilization of biomass and the purification of dye wastewater are urgent problems. In this study, a biomass aerogel (CaCO₃@starch/polyacrylamide/TEMPO-oxidized nanocellulose, CaCO₃@STA/PAM/TOCN) was prepared by combining nanocellulose with starch and introducing calcium carbonate nanoparticles, which exhibited a rich three-dimensional layered porous structure with a very light mass. Starch and nanocellulose can be grafted onto the molecular chain of acrylamide, while calcium carbonate nanopores can make the gel pore size uniform and have excellent swelling properties. Here, various factors affecting the adsorption behavior of this aerogel, such as pH, contact time, ambient temperature, and initial concentration, are investigated. From the kinetic data, it can be obtained that the adsorption process fits well with the pseudo-second-order. The Langmuir isotherm model can fit the equilibrium data well. The thermodynamic data also demonstrated the spontaneous and heat-absorbing properties of anionic and cationic dyes on CaCO₃@STA/PAM/TOCN aerogels. The adsorption capacity of Congo red (CR) and methylene blue (MB) by CaCO₃@STA/PAM/TOCN was 277.76 mg/g and 101.01 mg/g, respectively. Therefore, cellulose and starch-based aerogels can be considered promising adsorbents for the treatment of dye wastewater.