The
alluring properties of a luminescent graphene quantum dot (GQD)-based
nanocomposite are unquestionable to realize many advanced applications,
such as sweat pH sensors. The well-suited hydrophilic polymers to
host GQDs can face an unavoidable swelling behavior, which deteriorates
the mechanical stability, whereas the hydrophobic polymers can prevent
swelling but at the same time barricade the analyte pathways to GQDs.
To resolve the two aforementioned obstacles, we develop a nanocomposite
film containing nitrogen-doped GQDs (NGQDs) incorporated into a transparent,
elastic, and self-healable polymer matrix, composed of a hydrophobic n-butyl acrylate segment and a hydrophilic N-(hydroxymethyl)acrylamide segment for wearable healthcare pH sensors
on the human body. Besides serving as the fluorescence source, NGQDs
are also designed as a nano-cross-linker to promote abundant chemical
and physical interactions within the nanocomposite network. This synergetic
effect gives rise to a 10-fold higher mechanical strength, 7-fold
increment in Young’s modulus, 4-fold increment in toughness,
and 15-fold more sensitivity in pH detection (pH 3–10) compared
to those of the pristine copolymer and NGQDs, respectively. Moreover,
the mechanically enhanced nanocomposite possesses a high self-healing
efficiency (94%) at room temperature even under water and demonstrates
a stable sensing performance after repetitive usage for 30 days. Our
work provides insights into the simple preparation of human skinlike
nanocomposite elastomers usable for wearable pH sensors.