Modulation of Ice Formation and Removal Dynamics by Antifreeze Protein‐Inspired Large‐Area Films

ABSTRACT Artificial antifreeze strategies that regulate ice formation and removal are critical for applications in cryopreservation, energy, and transportation. Natural antifreeze proteins (AFPs) offer precise control over ice formation but suffer from poor scalability and environmental instability. Here, we report an AFP‐inspired large‐area film featuring programmable freezing dynamics and integrated photothermal de‐icing functionality. The films replicate AFPs’ dual‐face structure, graphene oxide with edge carboxyls/hydroxyls mimics the ice‐binding face (promoting nucleation). The films mimicking the non‐ice‐binding face are fabricated via coordination‐guided site‐selective removal of carboxyl groups, effectively reducing the C═O content to 0.42%. This structure endows the films with a freezing delay up to 2010 s and tunable freezing rates, achieved by tailoring laser‐treated patterns, allowing for precise control of ice formation. Due to their broadband absorption, enhanced photothermal conversion, and high thermal conductivity, the films efficiently remove ice and suppress frost under light exposure, even in freezing humid conditions, outperforming natural AFPs. As a demonstration, ultralight floating robots constructed from the films exhibit photothermal Marangoni propulsion and successfully navigate a maze under freezing conditions. This work highlights the potential of artificial photothermal antifreeze films for programmable ice control, anti‐icing, and soft robotics in extreme environments, surpassing the capabilities of natural AFPs.