Progress in the field of soft devices—that is, the types of haptic, robotic, and human-machine interfaces (HRHMIs) in which elastomers play a key role—has its basis in the science of polymeric materials and chemical synthesis. However, in examining the literature, it is found that most developments have been enabled by off-the-shelf materials used either alone or as components of physical blends and composites. A greater awareness of the methods of synthetic chemistry will accelerate the capabilities of HRHMIs. Conversely, an awareness of the applications sought by engineers working in this area may spark the development of new molecular designs and synthetic methodologies by chemists. Several applications of active, stimuli-responsive polymers, which have demonstrated or shown potential use in HRHMIs are highlighted. These materials share the fact that they are products of state-of-the-art synthetic techniques. The progress report is thus organized by the chemistry by which the materials are synthesized, including controlled radical polymerization, metal-mediated cross-coupling polymerization, ring-opening polymerization, various strategies for crosslinking, and hybrid approaches. These methods can afford polymers with multiple properties (i.e., conductivity, stimuli-responsiveness, self-healing, and degradable abilities, biocompatibility, adhesiveness, and mechanical robustness) that are of great interest to scientists and engineers concerned with soft devices for human interaction.