Inspired by the unfolding triggered crosslinking of proteins like fibronectin, we sought to develop a new method of installing mechanosensitivity within synthetic polymer networks. Recently, we developed organogels and hydrogels with mechano-responsive properties, both based on preformed diacrylate crosslinks with reactive pendent thiols for post-polymerization crosslinking. Both systems begin as a crosslinked network and respond to compression, strengthening several hundreds of kPa in elastic modulus over repeated cycles. The mechanosensitivity results from long PEG molecular shielding groups grafted to the polymer backbone, which prevent the reactive thiol groups from crosslinking until compression brings them together.