The physicochemical properties of rare-earth zirconates can be tuned by the rational modification of their structures and phase compositions. In the present work, La 3+ -, Nd 3+ -, Gd 3+ -, and Dy 3+ -zirconate nanostructured materials were prepared by different synthetic protocols, leading to powders, xerogels, and, for the first time, monolithic aerogels. Powders were synthesized by the co-precipitation method, while xerogels and aerogels were synthesized by the sol−gel technique, followed by ambient and supercritical drying, respectively. Their microstructures, thermogravimetric profiles, textural properties, and crystallographic structures are reported. The co-precipitation method led to dense powders (S BET < 1 m 2 g −1 ), while the sol−gel technique resulted in large surface area xerogels (S BET = 144 m 2 g −1 ) and aerogels (S BET = 168 m 2 g −1 ). In addition, the incorporation of lanthanide ions into the zirconia lattice altered the crystal structures of the powders, xerogels, and aerogels. Single-phase pyrochlores were obtained for La 2 Zr 2 O 7 and Nd 2 Zr 2 O 7 powders and xerogels, while defect fluorite structures formed in the case of Gd 2 Zr 2 O 7 and Dy 2 Zr 2 O 7 . All aerogels contain a mixture of cubic and tetragonal ZrO 2 phases. Thus, a direct effect is shown between the drying conditions and the resulting crystalline phases of the nanostructured rare-earth zirconates.