The growth of single crystals of the single layered manganites with compositions La1-xSr1+xMnO4 (0less than or equal toxless than or equal to0.6) by the floating zone technique is reported. Several neutron and X-ray scattering techniques were used to characterize the samples. Based on these data, the growth parameters were optimized with regard to structural (i.e. mosaic spread) and chemical homogeneity of the crystals. In addition, the neutron data show strong changes of the antiferromagnetic ordering as a function of the doping level x, i.e. upon increasing the mean Mn valence in La1-xSr1+xMnO4. (C) 2002 Elsevier Science B.V. All rights reserved.