Nature
has inspired the design of next-generation lightweight architectured
structural materials, for example, nacre-bearing extreme impact and
paw-pad absorbing energy. Here, a bioinspired functional gradient
structure, consisting of an impact-resistant hard layer and an energy-absorbing
ductile layer, is applied to additively manufacture ultrahigh-molecular-weight
polyethylene (UHMWPE). Its crystalline graded and directionally solidified
structure enables superior impact resistance. In addition, we demonstrate
nonequilibrium processing, ultrahigh strain rate pulsed laser shock
wave peening, which could trigger surface hardening for enhanced crystallinity
and polymer phase transformation. Moreover, we demonstrate the paw-pad-inspired
soft- and hard-fiber-reinforced composite structure to absorb the
impact energy. The bioinspired design and nonequilibrium processing
of graded UHMWPE shed light on lightweight engineering polymer materials
for impact-resistant and threat-protection applications.