The presence of organic pollutants in wastewater remains a prominent environmental concern due to the related ecological and health hazards. In response, this study employs an adsorptive methodology to address the removal of phenol and catechol, utilizing an organo-bentonite material modified with a pH-responsive switchable surfactant, dodecyldimethylamine oxide (C12DAO). The synthesized organo-bentonite (C12DAO-Bt) manifests commendable thermostability resulting from thermogravimetric analyses. The adsorption capacities of C12DAO-Bt concerning phenol and catechol intensify with the augmentation of the C12DAO/bentonite mass ratio. The utmost adsorption capacities of 150C12DAO-Bt, deduced through a pseudo-second-order kinetic model, stand at 5.72 mg·g−1 for phenol and 5.55 mg·g−1 for catechol, respectively. Subject to modification by a pH-responsive surfactant, conditions leaning towards weakly acidic and neutral conditions (pH = 6~7) are conducive to the adsorption of phenolic compounds. Conversely, alkaline conditions (pH = 8~9) facilitate the dissociation of adsorbates from adsorbents. The augmentation of cationic strength within the examined scope incites the adsorption procedure while impeding the desorption efficacy. In the case of cationic species with comparable ionic strengths, Na+ exhibited a superior effect on the adsorption–desorption dynamics of phenol, while Ca2+ exerts a more pronounced effect on those of catechol. Moreover, even following five consecutive acid–base regulation cycles, C12DAO-Bt retains a relatively high adsorption capacity and desorption efficacy, which underscores its exceptional regenerative capacity for removing phenolic compounds from wastewater.