Novel one-dimensional terbium 1,3,5-benzenetricarboxylate nanobelts have been synthesized on a large scale through direct precipitation in solution phase without the assistance of any surfactant, catalyst, or template. The as-obtained nanobelts present crystallinity in spite of the moderate reaction conditions, exhibiting 1D helical strands and a 3D network framework. The influence of the reaction temperature, concentration, molar ratio of reactants, and solvent on the belt-like nanostructure has been discussed in detail. A possible mechanism based on the crystal structure of the compound is proposed to account for the formation of the nanobelts. A detailed investigation of the photoluminescence of Tb(1,3,5-BTC)(H2O)·3H2O nanobelts indicates that the optical properties of these phosphors are dependent on their size. More interestingly, the luminescence color of the Tb(1,3,5-BTC)(H2O)·3H2O:Eu3+ nanobelts can be easily tuned from green to green-yellow, yellow, orange and red-orange due to the energy transfer from the Tb3+ to Eu3+ ions by changing the doping concentration of activator ions.