In the framework of the circular economy, spent coffee grounds were converted into powdered activated carbon by means of pyrolysis, using potassium hydroxide as the activating agent. Its adsorption capacity on a panel of phenolic compounds was compared with those of two commercial powdered activated carbons, after preliminary studies on organic dyes with different ionic properties, to assess the affinity between adsorbates and adsorbents. Pseudo-first-order and pseudo-second-order kinetic models were carried out, together with Freundlich and Langmuir isotherms. They were useful to calculate the breakthrough at 5%, 10%, and 50% of adsorption and the partition coefficients for the comparison of performance between different sorbent systems in a less biased manner (e.g., reducing bias associated with operational settings like sorbate concentration and sorbents dosage). The results showed that the removal efficiency for SCGs-AC was comparable with that of the commercial activated carbons with the highest partition coefficients for methylene blue (12,455 mg/g/μM, adsorption capacity = 179 mg/g) and 3-chlorophenol (81.53 mg/g/μM, adsorption capacity = 3765 mg/g). The lower efficiency in bromothymol blue and bisphenol-A adsorption was due to its different morphology and surface properties.