The demand for effective and long-term durable antibacterial
surfaces
has been ever-growing in the past decades. A wide variety of long-lasting
antibacterial surfaces developed from release-killing, active-killing,
and anti-fouling strategies have demonstrated the desired effectiveness
and durability so far. Most of these successful designs were developed
from toxic and fossil-based materials, which failed to comply with
the green design criteria. Furthermore, the longevity of these surfaces
remained an unaddressed challenge. Herein, we present a disruptive
paradigm that emphasizes both eco-friendliness and long-lasting antibacterial
properties. A bio-based active-killing essential oil, namely carvacrol,
and nonfouling carboxybetaine zwitterionic moieties were combined
and incorporated into a highly bio-based polyurethane (BPU). The long-lasting
active-killing property for this antibacterial BPU coating was enabled
through the extended release of the bounded carvacrol via hydrolysis
in an aqueous environment and compared to unbound carvacrol by liquid
infusion. Also, the release of carvacrol generates zwitterionic moieties
to prevent further bacterial attachment at the release site, resulting
in a “kill and defend” synergistic antibacterial function
in the BPU. The kinetics of the extended-release property were investigated
and compared with unbound carvacrol BPU coatings; unbound carvacrol
infused into BPU was quickly exhausted after 2 days of immersion in
water, while the extended-release surface exhibited a nearly constant
release rate of ∼128 ng cm–2 h–1 even after 45 days. The in vitro antibacterial
efficiency of the BPUs was quantitatively evaluated using the modified
ISO standard for cross-laboratory comparison. As a result, approximately
98.9 and 98.7% of Escherichia coli and Staphylococcus aureus were eliminated from the coating
surfaces, and only a negligible variance in the antibacterial efficiency
was observed after 5 cycles of test. The feasibility for practical
application was also demonstrated by challenging the BPU coatings
in everyday settings. This “built-to-last” design theory
provided insights for future development of greener antibacterial
coatings with long-term performance.