The binary phase diagram of the YAlO3 (YAP) - NdAlO3 (NAP) system was determined by differential thermal analysis (DTA) and X-ray powder diffraction (XRD) measurements. High purity nanocrystalline powders and small single crystals of Y_{1-x}Nd_{x}AlO_3 (0 ≤ x ≤ 1) have been produced successfully by modified sol-gel (Pechini) and micro-pulling-down methods, respectively. Both end members show high mutual solubility >25% in the solid phase, with a miscibility gap for intermediate compositions. A solid solution with x ≈ 0.2 melts azeotropic ca. 20 degrees below pure YAP. Such crystals can be grown from the melt without segregation. The narrow solid/liquid region near the azeotrope point could be measured with a "cycling" DTA measurement technique. ; Comment: 12 pages, 8 figures, submitted to J. Alloys. Compd