The proper application of millimeter-sized spherical porous ceramic supports in catalytic operations relies on their ease of handling, convenient separation, recyclability, high-catalyst-solid loading, and the optimum mass transfer of reactants and products. However, common granulation techniques of spherical carriers entail complex liquid-phase-based processes under severe conditions and the use of toxic or expensive reagents. The present study discusses the manufacturing of porous ceramic granules derived from an inexpensive silica source (diatomite, solid network) and a biopolymer cross-linked by ion exchange (sodium alginate, patterning structure). The results indicated that, with fixed granulation conditions, porous diatomite granules with a sphericity of approximately 0.9 could be successfully obtained by optimization of the diatomite/sodium alginate dispersion to a 30.07 wt.% solid content and 1560 mPa·s viscosity (at ~0.3 s⁻¹). Moreover, the described manufacturing process was proven effective in developing hierarchically porous diatomite granules that were heat-treated at 1200 °C with high sphericity (~0.9), acceptable compressive strength (5.17 ± 0.31 MPa), and porosity features (total porosity: 69.0 ± 2.9%, macropore size: 2.777 μm, mesopore size: 35.34 nm), establishing them as well-matched support materials for either catalytic or adsorption applications.