A novel method utilizing hydrocolloids to prepare nicely shaped spheres of metal-organic frameworks (MOFs) has been developed. Microcrystalline CPO-27-Ni particles are dispersed in either alginate or chitosan solutions, which are added dropwise to solutions containing, respectively, either divalent group 2 cations or base that act as gelling agents. Well-shaped spheres are immediately formed, which can be dried into spheres containing mainly MOF (>95 wt %). The spheronizing procedures have been optimized with respect to maximum specific surface area, shape, and particle density of the final sphere. At optimal conditions, well-shaped 2.5-3.5 mm diameter CPO-27-Ni spheres with weight-specific surface areas <10 % lower than the nonformulated CPO-27-Ni precursor, and having sphere densities in the range 0.8 to 0.9 g cm(-3) and particle crushing strengths above 20 N, can be obtained. The spheres are well suited for use in fixed-bed catalytic or adsorption processes.