Tartrate (Tar 2− ) was originally employed in this work as a chelating/structure-directing agent for hydrothermal crystallization of ZnWO 4 , where the decisive roles of Tar 2− /Zn 2+ /WO 4 2− molar ratio, solution pH (7−10), and the use of ethylene glycol (EG) cosolvent in phase/morphology evolution were deciphered in detail. It was unambiguously manifested that Tar 2− may remarkably retard the intrinsically preferred [001] growth of ZnWO 4 , transform 1D nanorods to 0D nanoparticles and then to 2D platelets, and meanwhile induce face-to-face alignment of the platelets to form spheroidal, ellipsoidal and snowflakelike 3D architectures, where the 2D crystallites were revealed to develop via oriented attachment (colattice) of non-(00l) facets. A lower solution pH and excessive WO 4 2− were clearly shown to enhance and offset the effect of Tar 2− , which led to ellipsoidal assemblies of substantially larger 2D crystallites and suppressed 2D growth/3D assembly of ZnWO 4 crystallites, respectively. With the spheroidal architectures for example, doping ZnWO 4 with RE 3+ yielded (Zn 0.98 RE 0.02 )WO 4 phosphors (RE = Sm, Eu, Tb, and Dy, respectively) that show luminescence overlapped from the typical linelike and broad-band (∼350−700 nm) emissions of RE 3+ and WO 6 , respectively. The luminescence color of the sample was found to drift away from the blue corner of the CIE chromaticity diagram with RE 3+ doping and to be dependent on the type of RE 3+ .