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Abstract Studying the behavior of anisotropic particles at fluid interfaces is a rapidly expanding field, as understanding how the introduced anisotropy affects the resulting properties is essential in the engineering of interfacial systems. Surface anisotropic particles, also known as Janus particles (JPs), offer new possibilities for novel applications due to their amphiphilicity and stronger binding to fluid interfaces compared to homogeneous particles. Introducing surface anisotropy creates complexity as the orientation of interfacially bound particles affects interparticle interactions, a contributing factor to the microstructure formation. In this work, we have investigated the microstructure of JP monolayers formed at the air–water interface using particles with different degrees of amphiphilicity and examined the response of the networks to applied compressions. Our findings demonstrate that JPs amphiphilicity is a crucial factor governing their orientation at the interface, which in turn dictates the complexity of the capillary interactions present and the mechanical properties of the ensuing networks.