Synergizing nanomaterial technology with advanced 3D printing techniques creates new opportunities for developing smart, stimuli-responsive materials suitable for tissue engineering scaffolds. By incorporation of stimuli-responsive nanoparticles into extracellular matrix mimetics, these composites gain functional elements capable of replicating dynamic biological processes in vitro. Herein, we propose combining hybrid multifunctional inorganic–organic materials with the emerging volumetric bioprinting (VBP) technique. We present two hybrid materials, a light stimuli-responsive polymer-based resin and a biocompatible porcine-derived decellularized extracellular matrix (dECM)-based bioresin, thus expanding the library of materials suitable for VBP. Plasmonic nanoparticles are combined with a thermoresponsive polymeric matrix, formulating the stimuli-responsive plasmonic resin, while a dECM-based bioresin with embedded smooth muscle cells (SMCs) is employed to include the biological component in the system. As proof of concept to demonstrate the versatility of the hybrid materials, we investigated the generation of highly complex structures, including multiwalled channels, using sequential VBP. Overall, this study broadens the range of materials compatible with VBP, thereby enabling the use of smart multicomponent materials in the fabrication of dynamic, stimuli-responsive 3D in vitro models.