In the pursuit of a more sustainable and climate-friendly future, there has been a notable boost in interest surrounding the application of electrochemistry. Owing to its heightened levels of control in terms of reaction rate and product selectivity over other approaches, electrocatalysis has carved out a distinct niche in the space of catalysis. Progress in sustainable electrocatalysis is inherently based on the development of efficient, non-noble metal-based electrode materials to not only diminish environmental impact but also increase their economic viability. Given the significant influence of electrode materials on the electron transfer rate and selectivity of a reaction, maximising their potential range and stability while minimising costs is paramount. Moreover, facile recyclability and reusability additionally favour the appeal of electrode materials. Rationalised design of such materials is essential for enhancing the aforementioned attributes and facilitating industrial-scale implementation. Surface-modification with macrocyclic molecules, such as cyclodextrins, calixarenes or pillararenes, offers a method for binding molecules through host-guest interactions. Such assemblies allow for the surface anchoring of molecular catalysts equipped with suitable binding units, such as naphthalene or adamantane groups. The anchoring of these catalysts through hydrophobic interactions enables their utilisation in electrochemical catalysis while maintaining their ability to be replaced with fresh catalyst molecules upon degradation. Surface-bound metal complexes have been shown to retain the high specific activity and selectivity of molecular species while also benefiting from inherent advantages of heterogeneous electrocatalysts including increased stability and reduced catalyst loading requirements. Furthermore, immobilised catalysts allow for reactions to be conducted in aqueous media, even when the catalyst itself is hydrophobic. This eliminates certain constraints in catalyst design, particularly by enabling the ligand sphere of a metal complex to be tuned to a specific reaction without solubility restrictions. Importantly, the dynamic equilibrium of host-guest complex formation, as observed in solution, is shifted significantly in favour of the host-guest complexes when the host is bound to a surface, which results in a more stable binding than expected from homogeneous experiments. Pillararenes show remarkable self-assembly characteristics in both solution and on surfaces, directly dependent on their ring size and level of functionalisation. Huang and co-workers pioneered surface-modification with pillararenes when investigating functionalised gold particles for their host-guest complexation behaviours as well as their ability to function as reaction cavities. In a subsequent development, Inagi and coworkers demonstrated the electrochemically induced oxidative generation of micron-sized hexagonal cylinders from pillar [6]arene (PA [6]) on indium tin oxide (ITO) electrodes. PA [6] are highly symmetric, hexagonally shaped macrocycles composed of six methylene-bridged 1,4-diphenol units, with the bridging units para to each other. With a cavity size of approximately 6.7 Å, they accommodate suitable guest species through hydrophobic, van der Waals, CH-π or π-π interactions. Strong binding is achieved with hydrocarbons, aromatic systems and cationic species. . Pillararene assemblies have since been explored across various domains, including but not limited to medicinal, sensing and catalysis applications, leveraging their ability to selectively uptake guest molecules based on their distinctive properties regarding size and degree of functionalisation. However, the functionalisation and adjustment of binding properties remains intricate, relying on sophisticated synthesis strategies. Here, we report the self-assembly of non-functionalised pillar [6]arenes on a mesoporous indium tin oxide (mITO) surface, serving as the working electrode for different electrocatalytically driven reactions involving three catalytically active ruthenium complexes as the guest molecules. The versatility, pH stability and reusability of such electrodes is demonstrated in the electrochemical oxidation of benzyl alcohol (pH 1-2.4) and ammonia (pH 10. 8-11.3).