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Neural implants that are based on mechanically adaptive polymers (MAPs) and soften upon insertion into the body have previously been demonstrated to elicit a reduced chronic tissue response than more rigid devices fabricated from silicon or metals, but their processability has been limited. Here we report a negative photoresist approach towards physiologically responsive MAPs. We exploited this framework to create cross-linked terpolymers of 2-hydroxyethyl methacrylate, 2-hydroxyethyl acrylate and 2-ethylhexyl methacrylate by photolithographic processes. Our systematic investigation of this platform afforded an optimized composition that exhibits a storage modulus E ′ of 1.8 GPa in the dry state. Upon exposure to simulated physiological conditions the material swells slightly (21% w/w) leading to a reduction of E ′ to 2 MPa. The large modulus change is mainly caused by plasticization, which shifts the glass transition from above to below 37 °C. Single shank probes fabricated by photolithography could readily be implanted into a brain-mimicking gel without buckling and viability studies with microglial cells show that the materials display excellent biocompatibility.