This work deals with promoting the efficiency of removing the cationic and ionic dyes by new aerogel–carbon nanostructures. For cleaner production the rice straw-pulping black liquors, which regards serious environmental risk during routine disposing, is used in preparing the aerogel precursors. These aerogels (AGBs) depend on using pulping black liquor in hybrid with resorcinol and the less carcinogenic formaldehyde butyraldehyde. Black liquors from five pulping processes are used, Elemental, thermogravimetric (TGA and DTG), and FTIR-ATR analyses are used to characterize the carbon precursors. While their adsorption behavior toward cationic and anionic dyes are accessed via iodine-value, adsorption capacity and kinetic models, textural characterization, and SEM. The TGA measurements reveal that AGBs from BLs of neutral sulfite and soda-borohydride pulping reagents have higher activation and degradation energies than other aerogels. In terms of cationic and anionic dyes adsorption as well as textural characterization, the AGB-CNSs surpass that made from BLs. The discarded KOH/NH4OH black liquor is used to synthesize the best aerogel precursor for producing cationic methylene blue dye (MB) adsorbent, where it provides an adsorption capacity 242.1 mg/g. The maximum anionic brilliant blue dye (BB) adsorption capacity, 162.6 mg/g, is noticed by Kraft BL-aerogel-CNSs. These finding data overcome the literature carbon adsorbents based on lignin precursors. All examined CNSs toward MB dye follow the Langmuir adsorption equilibrium; while primarily the Freundlich model for BB dye. The pseudo-second-order kinetic model well fits the adsorption kinetics of investigated AGB-CNSs. The textural characterization and SEM revealed a mixture of mesoporous and micro porous features in the CNSs.