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Abstract Crosslinking is a ubiquitous strategy in polymer engineering to increase the thermomechanical robustness of solid polymers but has been relatively unexplored in the context of π‐conjugated (semiconducting) polymers. Notwithstanding, mechanical stability is key to many envisioned applications of organic electronic devices. For example, the wide‐scale distribution of photovoltaic devices incorporating conjugated polymers may depend on integration with substrates subject to mechanical insult—for example, road surfaces, flooring tiles, and vehicle paint. Here, a four‐armed azide‐based crosslinker (“4Bx”) is used to modify the mechanical properties of a library of semiconducting polymers. Three polymers used in bulk heterojunction solar cells (donors J51 and PTB7‐Th, and acceptor N2200) are selected for detailed investigation. In doing so, it is shown that low loadings of 4Bx can be used to increase the strength (up to 30%), toughness (up to 75%), hardness (up to 25%), and cohesion of crosslinked films. Likewise, crosslinked films show greater physical stability in comparison to non‐crosslinked counterparts (20% vs 90% volume lost after sonication). Finally, the locked‐in morphologies and increased mechanical robustness enable crosslinked solar cells to have greater survivability to four degradation tests: abrasion (using a sponge), direct exposure to chloroform, thermal aging, and accelerated degradation (heat, moisture, and oxygen). 

Haptic devices are in general more adept at mimicking the bulk properties of materials than they are at mimicking the surface properties. Herein, a haptic glove is described which is capable of producing sensations reminiscent of three types of near‐surface properties: hardness, temperature, and roughness. To accomplish this mixed mode of stimulation, three types of haptic actuators are combined: vibrotactile motors, thermoelectric devices, and electrotactile electrodes made from a stretchable conductive polymer synthesized in the laboratory. This polymer consists of a stretchable polyanion which serves as a scaffold for the polymerization of poly(3,4‐ethylenedioxythiophene). The scaffold is synthesized using controlled radical polymerization to afford material of low dispersity, relatively high conductivity, and low impedance relative to metals. The glove is equipped with flex sensors to make it possible to control a robotic hand and a hand in virtual reality (VR). In psychophysical experiments, human participants are able to discern combinations of electrotactile, vibrotactile, and thermal stimulation in VR. Participants trained to associate these sensations with roughness, hardness, and temperature have an overall accuracy of 98%, whereas untrained participants have an accuracy of 85%. Sensations can similarly be conveyed using a robotic hand equipped with sensors for pressure and temperature.