In this work, spent coffee grounds (SCG) were treated using sulfuric acid hydrolysis in order to isolate the sulfuric acid lignin (SAL). The reactivity of SAL was improved through phenolation and acetylation. Spectroscopic analysis showed that the isolated lignin is composed of GHS type and it was characterized by a high amount of (C-C) and β-O-4 bonds. The thermal analysis showed that the phenolated sulfuric acid lignin (Ph-SAL) present higher thermal stability compared to SAL and acetylated sulfuric acid lignin. In addition, the phenolic hydroxyl group content increases from 2.99 to 9.49 mmol/g after phenolation. Moreover, a methylene blue (MB) adsorption test was established in order to find out the sorption capacity of different samples. The study showed that the adsorbed amount of dye increase after the chemical modification of SAL, especially after phenolation. The removal efficiency was enhanced after modification to reach 99.62% for Ph-SAL. The evaluation of the adsorption experimental data with the theoretical models of Langmuir and Freundlich showed that the best fitting was expressed by the Langmuir model for all samples. Finally, this study showed that lignin isolated from SCG can be simply and easily chemical modified and exhibits excellent adsorption ability towards cationic dyes (MB) in aqueous solutions. As a renewable, low-cost, and natural biomass material, lignin from SCG shows a promising practical and economical application of biomass in the field of wastewater purification.