In contemporary applications, smart surfaces capable
of altering
their properties in response to external stimuli have garnered significant
attention. Nonetheless, the efficient creation of smart surfaces exhibiting
robust and rapid responsiveness and meticulous controllability on
a large scale remains a challenge. This paper introduces an innovative
approach to fabricate smart surfaces with strong pH-responsiveness,
combining femtosecond laser direct writing (LDW) processing technology
with stimulus-responsive polymer grafting. The proposed model involves
the grafting of poly(2-diethylaminoethyl methacrylate) (PDEAEMA) onto
rough and patterned Au/polystyrene (PS) bilayer surfaces through Au-SH
bonding. The incorporation of LDW processing technology extends the
choice of microstructures and roughness achievable on material surfaces,
while PDEAEMA imparts pH responsiveness. Our findings revealed that
the difference in contact angle between acidic and basic droplets
on the rough PDEAEMA-g-Au surface (∼118°)
greatly surpasses that on the flat PDEAEMA-g-Au surface
(∼72°). Next, by leveraging the precision control over
surface microstructures enabled by the LDW processing technique, this
difference was further augmented to ∼127° on the optimized
patterned PDEAEMA-g-Au surface. Further, we created
two distinct combined smart surfaces with varying wettability profiles
on which the hydrophilic–hydrophobic boundaries exhibit reliable
asymmetric wettability for acidic and basic droplets. Additionally,
we prepared a separator, realizing a better visual distinction between
acid and base and collecting them separately. Given the effective
abilities found in this study, we postulate that our smart surfaces
hold substantial potential across diverse applications, encompassing
microfluidic devices, intelligent sensors, and biomedicine.