The production of high-quality phosphors for white-emitting applications is an important goal for the settlement of light-emitting diodes (LEDs) in the market and households. Single phosphors directly yielding white emission are advantageous in comparison to a mixture of individual red, green, and blue phosphors as these are hampered by reabsorption of the blue light. Here, a combined approach to uniform, nanoscale particles as single-white-emitting phosphor is realized via an ionic-liquid-based synthesis. LaF3 particles codoped with various amounts of Tm3+, Tb3+, and Eu3+ were synthesized, and their structural, morphological, and optical properties were studied. Small particles with a mean size of 6–8 nm were obtained with a narrow size distribution. At small dopant ion concentrations, white light emission close to standard daylight D65 is obtained under excitation of λex = 355 nm where simultaneous emissions of all three optically active ions occur.