With the development of biomedical engineering, the preparation
of hydrogels with combined extreme mechanical properties similar to
those of some biological hydrogels becomes an important research topic
for scientists. In this work, a single-network hydrogel with combined
extreme mechanical properties is prepared through a simple and universal
method, wherein the strength, elongation at break, toughness, and
fracture energy of the hydrogel WPU-3PAAm-6PAN are achieved at 24.7
MPa, 544.0%, 68.9 MJ m–3, and 37.2 kJ m–2, respectively. Herein, a series of photosensitive resins in emulsion
form are synthesized, and due to the water–oil diphasic characteristic,
hydrophobic monomers and high-efficient hydrophobic photo-initiators
are adopted into the resins, which can significantly improve the mechanical
properties of the hydrogels due to the hydrophobic association effect
and solve the biggest barrier of low curing rate in digital light
processing (DLP) fabrication of hydrogels, respectively. Moreover,
the simple and facile method to obtain robust and tough hydrogels
can be universally applied to other polymer systems. Combined with
the excellent mechanical properties and printing ability, the hydrogels
with optimized structures are fabricated through DLP printing technology
and applied as tendon substitutes. The tendon substitutes exhibit
superior performance for mechanical connection and regeneration of
collagen fibers. Although further clinical research is required, the
hydrogels have great potential applications in various biological
areas.