  Photoinduced network formation is an attractive strategy for designing
water-insoluble gelatin fibres as medical device building blocks and for
enabling late-stage property customisation. However, mechanically-competent,
long-lasting filaments are still hard to realise with current photoactive, e.g.
methacrylated, gelatin systems due to inherent spinning instability and
restricted coagulation capability. To explore this challenge, we present a
multiscale approach combining the synthesis of 4-vinylbenzyl chloride
(4VBC)-functionalised gelatin (Gel-4VBC) with a voltage-free spinning and
UV-curing process so that biopolymer networks in the form of either individual
fibres or nonwovens could be successfully manufactured. In comparison to
state-of-the-art methacrylated gelatin, the mechanical properties of UV-cured
Gel-4VBC fibres were readily modulated by adjustment of coagulation conditions,
so that an ultimate tensile strength and strain at break of up to ~80 MPa and
~9 % were measured, respectively. The sequential functionalisation /spinning
route proved to be highly scalable, so that one step spunlaid formation of
fibroblast-friendly nonwoven fabrics was successfully demonstrated with wet
spun Gel-4VBC fibres. The presented approach could be exploited to generate a
library of gelatin building blocks tuneable from the molecular to the
macroscopic level to deliver computer-controlled extrusion of fibres and
nonwovens according to defined clinical applications.
