Reported approach aims for the synthesis of spherical cellulose beads with high production rates (0.7–4.1 kg/h of hydrogel) via the so-called jet cutting method. To form particles, jets of aqueous cellulose/sodium hydroxide solutions were cut into pieces and collected in a gelation bath (30 wt% aqueous H2SO4, 20 °C). After solvent exchange with ethanol and subsequent supercritical drying, cellulose aerogel particles were obtained. The particles showed high specific surface areas (ca. 400 m2/g) and low bulk (untapped) densities (0.06–0.10 g/cm3). Variation of cellulose content (4–7 wt%) and jet cutting process parameters (cutting frequency, nozzle diameter, jet velocity) turned to be useful parameters for controlling the particles size and shape. Highly spherical particles with sphericity SPH ≥ 0.92 were obtained in a broad range of achievable particle sizes (0.4–1.0 mm), with an optimum of SPH at 6 wt% cellulose content.