In this article, we present a simple, advanced method to produce lightweight tailor-made materials based on capillary suspensions that are made from locally bonded hollow glass spheres with a high total porosity in the range of 70% at apparent densities of 200 kg/m3, having a compressive strength of 0.6 MPa. The amount of added liquid and the particle surface treatment determine the network structure in the pastes and the resulting microstructure of the porous material in a straightforward manner. This structure has a strong impact on the porosity, pore size, and mechanical properties of the final body. The most promising porous materials were made of surface treated hollow glass spheres that create a sample-spanning network in the capillary state, where the added liquid wets the particles worse than the bulk fluid. These samples approach the density of natural balsa wood and they may find application in fields where either weight or structure are important, such as in insulation materials, filters, and membranes, as well as lightweight construction materials for automotive or aerospace engineering.