We have grown cubic centimeter-size crystals of YBa2Cu3O, suitable for neutron studies, by a top-seeded melt-growth technique. Growth conditions were optimized with an eye toward maximizing phase purity. It was found that the addition of 2% Y2BaCuO5 and 0.5% Pt (by mass) were required to prevent melt loss and to obtain the highest crystallinity. A neutron diffraction study on a mosaic of six such crystals found that the final Y2BaCuO5 concentration was 5%, while other impurity phases comprised less than 1% by volume. The oxygen content was set to x = 6.5, the crystals were detwinned, and then carefully annealed to give the well-ordered ortho-II phase. The neutron study determined that 70% of the mosaic's volume was in the majority orthorhomic domain. The neutron (006) and (110) rocking curve widths were similar to1degrees per crystal and similar to2.2degrees for the mosaic, and the oxygen chain correlation lengths were >100 Angstrom in the a- and b-directions and similar to50 Angstrom in the c-direction.