Abstract Additive manufacturing permits innovative soft device architectures with micron resolution. The processing requirements, however, restrict the available materials, and joining chemically dissimilar components remains a challenge. Here we report silicone double networks (SilDNs) that participate in orthogonal crosslinking mechanisms—photocurable thiol-ene reactions and condensation reactions—to exercise independent control over both the shape forming process (3D printing) and final mechanical properties. SilDNs simultaneously possess low elastic modulus ( E 100%  < 700kPa) as well as large ultimate strains (d L/L 0 up to ~ 400 %), toughnesses ( U ~ 1.4 MJ·m −3 ), and strengths ( σ ~ 1 MPa). Importantly, the latent condensation reaction permits cohesive bonding of printed objects to dissimilar substrates with modulus gradients that span more than seven orders of magnitude. We demonstrate soft devices relevant to a broad range of disciplines: models that simulate the geometries and mechanical properties of soft tissue systems and multimaterial assemblies for next generation wearable devices and robotics.