Single crystals of a bilayer manganite series Pr(Sr1-xCax)(2)Mn2O7 (x=0, 0.4, 0.9, 1) have been grown using traveling solvent floating zone technique under various oxygen partial pressure. It was found that the crystal quality is very sensitive to oxygen partial pressure applied during growth and highly Ca doped crystals could only be obtained at elevated oxygen pressure. Whereas a secondary phase was observed for PrCa2Mn2O7 grown at oxygen partial pressure below 1 bar, a pure phase can be achieved at 8 bar of oxygen. This was evidenced studying composition mapping by X-ray fluorescence spectroscopy. X-ray Laue diffraction and X-ray powder diffraction have been carried out on the samples for the quality check of the grown crystals. Susceptibility measurements indicate that all samples are antiferromagnetic at low temperature. They also reveal the existence of two anomalies at similar to 320 K and 370 K, which coincide with the charge ordering/orbital ordering transitions described in the literature. (C) 2012 Elsevier B.V. All rights reserved.