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Abstract Biofouling at the solid–liquid–air interface poses a serious threat to public health and environmental sustainability. Despite the variety of antifouling materials developed, few have proven to resist fouling at the three‐phase contact line. In fact, antifouling at the liquid–solid interface and the air–solid interface call for opposite surface properties—hydrophilic for the former and hydrophobic for the latter. By devising a new design strategy, one that maximizes the mismatch of surface energies of comonomers for dynamic chain reorientation at the three‐phase contact line, an antifouling amphiphilic copolymer is obtained. The novel amphiphilic copolymer reduces the formation of biofilms byPseudomonas aeruginosaand outperforms a zwitterionic polymer, the current leading antifouling chemistry. The copolymer is synthesized using initiated chemical vapor deposition (iCVD), which leads to molecular‐level heterogeneities composed of zwitterionic and fluorinated moieties by avoiding undesirable surface tension effects. Atomic force microscopy, x‐ray diffractometry, and Fourier transform infrared spectroscopy confirm the copolymer's amphiphilicity and lack of microphase separation. Scanning electron microscopy provides visual confirmation of the diminished biofilm growth. The versatile iCVD technique is amenable to a range of substrates and enables the application of this new material to food processing, healthcare, and underwater performance.