Hypothesis: The anisotropic nature of colloidal particles results in orientation-dependent interactions that organize the particles into peculiar structures different from those formed by isotropic colloids. Particles with a hydrophilic hemisphere are expected to assemble in hydrophobic solvents due to the contribution of hydrophobic interactions as observed for molecular amphiphiles . Experiments: Asymmetrically decorated silica-based Janus particles are dispersed in an apolar solvent, chloroform, and their structure and dynamics are studied by light scattering and compared with computer simulations. Findings: Gelation of amphiphilic Janus particles with asymmetric surface decoration is observed in a hydrophobic medium. The influence of particle asymmetry on gel structure and dynamics is discussed. Unlike particles with long-range repulsive interactions in water, these systems rapidly form rather compact structures that are nevertheless more ramified than those made of isotropic hydrophobic particles. Comparison with computer simulations allows visualization of the gel and reveals a contribution of asymmetric short-range attractions and cross-term repulsions to the net effective interaction potential. (c) 2021 Elsevier Inc. All rights reserved.