Polymer
hydrogels, water-laden 3D cross-linked networks, find broad
application as advanced biomaterials and functional materials because
of their biocompatibility, stimuli responsiveness, and affordability.
The cross-linking density reports material properties such as elasticity,
permeability, and swelling propensity. However, this critical design
parameter can be challenging to template locally. Here, we report
a continuous processing scheme that uses laminar flow to direct the
organization of cross-linking density across a single sample. Dilute
and concentrated poly(ethylene glycol) diacrylate solutions are fed
into custom serpentine millifluidic devices. These feature a modular
sequence of splitting, rotation, and recombination elements, which
create patterned streamlines that serve as a template for hierarchical
concentration distributions. Poly(acrylic acid) microgels impart viscoplasticity,
which stabilizes layered flow during multiplication and ensures reliable
advection. The devices produce structured, seamless filaments, which
are then arranged into objects using 3D printing, and photopolymerized
to secure the heterogeneous distribution. The flow-encoded, multiscale
architecture provides mechanical contrast, which is demonstratively
exploited to program robust and reversible shape transformations,
potentially useful in soft actuator and sensor applications. The unique
structures achieved, and the geometrically dictated, chemistry-agnostic
operating principles used to achieve them, provides a new means to
engineer hydrogels to suit a variety of applications.