Nanosized sorbents are widely used for uranium (VI) recovery due to their high specific surface area, but the research on the integration of micromotors with nanosorbents to establish self-locomotive composites is still worth exploring. Thus, self-locomotive composites PS@PDA@Ag/SiO2-AO (PPA/SA) based on asymmetric micromotors and covalently attached nanosorbents were designed for selective uranium recovery. Pickering emulsion, as an important micro-reactor, was firstly adopted to prepare Janus microspheres with chemically distinct structure (PS@PDA@Ag), on which one hemisphere was loaded with catalytic silver (Ag) nanoparticles. Then, amidoxime (AO) decorated SiO2 nanospheres were covalently attached onto another hemisphere of PS@PDA@Ag, anisotropic configuration of as-prepared PPA/SA avoided the overlap of catalytic and binding sites. The self-propelled motion of PPA/SA induced by asymmetrical bubble evolution by H2O2 was observed, and the maximum speed was about 25 μm s−1 in case of 5 % H2O2. The uranium adsorption onto PPA/SA achieved 92 % of the equilibrium amount (29.31 mg g−1) in the first 20 min, and this value increased to 38.71 mg g−1 under the condition of H2O2, suggesting that autonomous movement achieves rapid mixing and mass transportation. The maximum adsorption amount (Qm) is 114.0 mg g−1 at 298 K according to the Langmuir model. In addition, PPA/SA exhibited remarkable selectivity for uranium even in the presence of large amounts of Na+, Mg2+, K2+, Ca2+ and other ions in the simulated seawater solution.