Self-assembled unusual ZnO ellipsoids have been grown by a facile low-temperature (60 degrees C) solution process on a large scale. FESEM and TEM reveal that these ellipsoids have an average horizontal axis of 1.5 mu m and a longitudinal axis of 0.6 mu m. Experimental results obtained from the early growth stage demonstrate that the ZnO ellipsoidal structures are single crystals and formed from direct "oriented attachment" of two types of building blocks, that is, nanorods and nanoparticles. It is further found that the existence of poly( ethylene glycol) (PEG-10 000) is vital to the formation of the complex microparticles. Raman spectrum, room-temperature photoluminescence, and UV-vis absorption spectra are also discussed. This work presents a simple and effective route for large-scale fabrication of single-crystal ZnO ellipsoids with micrometer-scale sizes and 3D self-assembled structures.