We report the fabrication of clay-mineral-based Janus microspheres that exhibit remotely steerable self-propulsion in water, facilitating their selective and active removal of radiocesium from a contaminated solution. The spray-drying of slurries of intrinsically Cs-selective illite containing iron oxide nanoparticles led to magnetic illite microspheres with superior Cs adsorption capability and superparamagnetic behavior. The Janus micromotor adsorbent was prepared by depositing catalytic Pt onto the half-surface of magnetic illite microspheres. The micromotor adsorbents exhibited self-propulsion at speeds as high as ~265 µm/s via asymmetric bubble generation in water containing HO as a fuel. The self-propulsion of the adsorbent improved the Cs adsorption kinetics six-folds compared with the kinetics in the corresponding stationary liquid. The magnetic properties of the micromotor adsorbent enabled convenient separation and direction control of the adsorbents under an external magnetic field. In particular, the micromotor adsorbent could successfully remove more than 98.6% of Cs from aqueous media containing competing ions including K, Na, Ca and Mg.