Self-assembled covalent-organic frameworks (COFs) are a cutting-edge approach for exploring novel magnetic properties due to their well-defined, two-dimensional structures and customizable chemical environments. Their unique geometry supports the study of frustrated magnetism, where competing interactions hinder the system from minimizing all forces simultaneously, leading to intriguing quantum spin liquid (QSL) phases. These phases are promising for quantum computing due to their potential for robust qubits and fault-tolerant computation. Unlike bulk materials or multilayer structures, which often face challenges such as uncontrollable defects that can quench quantum properties, COFs on surfaces offer an ideal platform. They provide precise control over lattice symmetry and magnetic interactions while avoiding synthesis complexities and defects. This proposal aims to advance research by developing a novel COF with a frustrated Kagomé-honeycomb (KH) lattice. The originality of this approach lies in combining surface-supported COF synthesis with innovative methods for tuning frustrated magnetism. Specifically, an organic radical linker covalently bonded with inorganic molecular magnets allows for precise tuning of exchange interactions. This is achieved by controlling the spatial overlap between the radical and metal centers through fine-tuning the noble metal substrate’s work function via chemical passivation, enabling reversible switching between different charge states of the radical linker. By creating a model system for controlling magnetic interactions, this approach enhances our ability to manipulate frustrated magnetic ground states on surfaces. It opens new avenues for understanding magnetism and chemistry, with potential applications in topological quantum computing, data storage, and spintronic devices.