In the paper, the materials ScPO4 center dot 2H(2)O and ScPO4 with multiform morphologies of spherical-like, flowerlike and regular tetrahedron micro-crystals as well as dispersive nano-particles, have been synthesized via a facile and controllable hydrothermal route assisted by the different organic additives under the different pH values. The scanning electron microscope and transmission electron microscopy results indicate that all of the pH value, the chelating agent, surfactant and solvent composition have obvious effects on the morphologies of samples, especially the pH value and the chelating agent. According to the density-functional theory, the band gap of ScPO4 is calculated as about 4.4 eV. After the active ions Tb3+ and Yb3+ are introduced into the host, ScPO4: Tb3(+,) Yb3+ presents the excellent multicolor optical properties in the photoluminescence, cathodoluminescence and up-conversion luminescence regions and based on the energy level schematic the luminescence mechanism is carefully investigated. All the results imply that the ability to generate ScPO4 nano/micro-crystals with the multiform morphologies and tunable emission colors provides a great opportunity for systematically evaluating their synthesis routes, as well as fully exploring their applications in many types of color display fields. (C) 2016 Elsevier B.V. All rights reserved.