Objects floating at a liquid interface, such as breakfast cereals floating in a bowl of milk or bubbles at the surface of a soft drink, clump together as a result of capillary attraction. This attraction arises from deformation of the liquid interface due to gravitational forces; these deformations cause excess surface area that can be reduced if the particles move closer together. For micrometer-sized colloids, however, the gravitational force is too small to produce significant interfacial deformations, so capillary forces between spherical colloids at a flat interface are negligible. Here, we show that this is different when the confining liquid interface has a finite curvature that is also anisotropic. In that case, the condition of constant contact angle along the three-phase contact line can only be satisfied when the interface is deformed. We present experiments and numerical calculations that demonstrate how this leads to quadrupolar capillary interactions between the particles, giving rise to organization into regular square lattices. We demonstrate that the strength of the governing anisotropic interactions can be rescaled with the deviatoric curvature alone, irrespective of the exact shape of the liquid interface. Our results suggest that anisotropic interactions can easily be induced between isotropic colloids through tailoring of the interfacial curvature.olloidal self-assembly is a promising route toward the fabrication of new nano-and microstructured materials (1-3). Interesting superstructures can be obtained provided that the particle-particle interactions can be controlled, both in strength and in directionality. Recent examples include the formation of well-defined clusters (4, 5) or complex colloidal crystals (5, 6) using particles decorated with sticky patches. Many strategies to achieve directional interaction potentials rely on the use of anisometric particles, or particles that have patches of distinct chemical functionality at their surface (7,8). Although effective, such particles are difficult to produce and typically only in low yields. Inducing anisotropic interactions between isotropic spherical particles requires the imposition of a directional external field or template; this has been achieved through application of electric or magnetic fields (9) or by immersing the particles in anisotropic fluids (10). Although liquid interfaces could be ideally suited as a template for self-assembly of nanoparticles or colloids (11-15), control of the directionality of the interactions is still lacking.Colloidal particles adsorb strongly to the interface between two immiscible fluids, driven by a reduction of the interfacial area. For micrometer-sized colloids, the adsorption energy can be as large as 10 7 times the thermal energy kT, making particle adsorption essentially irreversible. The lateral organization of the particles at the interface is determined by interparticle interactions. Isotropic repulsion, for example by electrostatic forces, leads to crystallization into a hexagonal lattice...