A massive carbon
footprint is associated with the ubiquitous use
of plastics and their afterlife. Greenhouse gas (GHG) emissions from
plastics are rising and increasingly consuming the global “carbon
budget”. It is, hence, paramount to implement an effective
strategy to reclaim postconsumer plastic as feedstock for technologically
innovative materials. Credible opportunity is offered by advances
in materials chemistry and catalysis. Here, we demonstrate that by
dynamically crosslinking thermoplastic polyolefins, commodity plastics
can be upcycled into technically superior and economically competitive
materials. A broadly applicable crosslinking strategy has been applied
to polymers containing solely carbon–carbon and carbon–hydrogen
bonds, initially by maleic anhydride functionalization, followed by
epoxy–anhydride curing. These dynamic networks show a distinct
rubber modulus above the melting transition. We demonstrate that sustainability
and performance do not have to be mutually exclusive. The dynamic
network can be extruded into a continuous filament to be in three-dimensional
(3D) printing of complex objects, which retain the mechanical integrity
of vitrimers. Being covalently crosslinked, these networks show a
thermally triggered shape-memory response, with 90% recovery of a
programmed shape. This study opens up the possibility of reclaiming
recycled thermoplastics by imparting performance, sustainability,
and technological advances to the reprocessed plastic.