This research proposes the application of iron-loaded sepiolite (S-Fe) as a catalytic adsorbent for the unreported 1-butylpyridinium chloride ([bpy] Cl) treatment in an aqueous medium. Initially, sepiolite was selected as an inexpensive and efficacious adsorbent for [bpy] Cl elimination. After that, sepiolite was loaded with iron for the subsequent electro-Fenton (EF) regeneration treatment. Once kinetic and isotherm studies were performed, providing respectively almost instantaneous adsorption (20 min) and an uptake of 22.85 mg/g, [bpy] Cl adsorption onto S-Fe was studied in continuous mode. The obtained breakthrough curve was analyzed using three standard breakthrough models, being Yoon–Nelson and Thomas the most suitable adjustments. Afterwards, S-Fe regeneration by the EF process was conducted using this iron-loaded silicate material as a heterogeneous catalyst. Under optimized operational conditions (current intensity 300 mA and Na2SO4 0.3 M), complete adsorbent regeneration was achieved in 10 h. The total mineralization of [bpy] Cl was reached within 24 h and among seven carboxylic acids detected, oxalic and acetic acids seem to be the primary carboxylic acids produced by [bpy] Cl degradation. Finally, S-Fe was efficiently used in four consecutive adsorption–regeneration cycles without a noticeable reduction in its adsorption capacity, opening a path for future uses.