Stable three-dimensional colloidal crystals were fabricated in an aqueous suspension of Tris buffer at pH > 8. The basic building blocks of the crystals were submicron-sized polystyrene-polyglycidol core-shell particles (Dn(SEM) = 270 ± 18 nm) with covalently bound 3,4-dihydroxyphenylalanine (l-DOPA). The growth of the crystals was triggered by a thermodynamically favorable arrangement of particles leading to their close packing and by the formation of covalent cross-links between the individual particles. Under alkaline conditions, molecules of l-DOPA are oxidized, which allows their participation in cross-linking, necessary for the stabilization of the formed colloidal crystals. The average size of the fabricated colloidal crystals is determined by their weight, density of the suspending medium, and the energy of their Brownian motion. Crystals generated during the suspension of particles fall down after reaching the critical weight. Therefore, crystals of similar dimensions are deposited at the bottom of the vessel. The described system is the first example of the formation of stable colloidal crystals in a suspension.