Paste-based printing is an additive manufacturing technique for fabricating multicomponent polymer-inorganic composites from air and photo curable pastes, which are extruded through a nozzle and then cured in a controlled fashion. A variety of active materials, such as surface functionalized silica and silicate nanoparticles, dyes, and chemically modified graphene platelets, mixed with commercially available silicone can be used to 3D print structures with on-demand mechanical, optical and electric properties. This work includes the development of ‘new chemistries’ for optimal incorporation of active materials at high mass loading (5-50 wt%) with appropriate rheological properties suitable for paste-printing. Examples of printed structures and devices include (i) photo-chromic, electro-chromic and thermo-chromic windows, (ii) high-strength composites, (iii) multifunctional metamaterials and (iv) thermal and corrosion barriers for electronic components. The multifaceted capabilities as demonstrated in this work, provides new perspectives for adoption of paste-printing as a versatile process towards fabrication of devices and parts for engineering and technological applications.