We report on controlled synthesis of uniform LnVO(4) (Ln = Ce and Nd) nanocrystals (NCs) with square-plate and H-shaped morphologies in nanosized reverse microemulsion reactors, via a facile solvo/ hydrothermal strategy. The NCs were thoroughly characterized by X-ray diffraction, transmission electron microscopy (TEM), atomic force microscopy (AFM), energy-dispersive X-ray spectroscopy (EDS), infrared absorption spectroscopy, and photoluminescence. Possible mechanisms of the rare-earth orthovanadate NC growth and size and shape evolution are proposed. A unique upconverted avalanche luminescence property pertaining to the NCs has been discovered, systematically studied, and mechanistically discussed. Our work combines synthetic and optical studies of the NCs and lays a foundation for reinventing their applications in optoelectronics among others.