Floating zone crystal growth and magnetic properties of bilayer manganites Pr(Sr1−xCax)2Mn2O7

► Phase-pure multiferroic single crystals of Pr(Sr1−xCax)2Mn2O7 were grown by floating zone method. ► Oxygen pressure was found critical to grow PrCa2Mn2O7 crystal. ► Composition homogeneity by crystal samples show by X-ray fluorescence spectroscopy mapping. ► Two charge/orbital ordering transitions were found in the temperature dependency of susceptibility.