Exploiting Molecular Dynamics in Composite Coatings to Design Robust Super‐Repellent Surfaces

Fluorinated motifs are promising for the engineering of repellent coatings, however, a fundamental understanding of how to effectively bind these motifs to various substrates is required to improve their stability in different use scenarios. Herein, the binding of fluorinated polyhedral oligomeric silsesquioxanes (POSS) using a cyanoacrylate glue (binder) is computationally and experimentally evaluated. The composite POSS–binder coatings display ultralow surface energy (≈10 mJ m(−2)), while still having large surface adhesions to substrates (300–400 nN), highlighting that super‐repellent coatings (contact angles >150°) can be readily generated with this composite approach. Importantly, the coatings show super‐repellency to both corrosive liquids (e.g., 98 wt% H(2)SO(4)) and ultralow surface tension liquids (e.g., alcohols), with ultralow roll‐off angles (<5°), and tunable resistance to liquid penetration. Additionally, these coatings demonstrate the potential in effective cargo loading and robust self‐cleaning properties, where experimental datasets are correlated with both relevant theoretical predictions and systematic all‐atom molecular dynamics simulations of the repellent coatings. This work not only holds promise for chemical shielding, heat transfer, and liquid manipulations but offers a facile yet robust pathway for engineering advanced coatings by effectively combining components for their mutually desired properties.