Ultrathin lanthanide (Nd, Pr, Eu, Sm) oxide films with functional dielectric properties down to 3.3 nm thickness were deposited by aqueous chemical solution deposition (CSD) onto hydrophilic SiO2/Si substrates. Precursor solutions were prepared from the oxides via an intermediate, solid Ln(III)citrate. A film heat treatment scheme was derived from thermogravimetric analysis of the precursor gels, showing complete decomposition by 600 °C. Crystalline phase formation in the films depended on the lanthanide, annealing temperature, and citric acid content in the precursor. Through variation of the precursor concentration and number of deposited layers, thickness series of uniform films were obtained down to ∼3 nm. The film uniformity was demonstrated both by atomic force microscopy and cross-section transmission electron microscopy. The lanthanide oxide films possessed good dielectric properties. It was concluded that aqueous CSD allows deposition of uniform ultrathin films and may be useful for the evaluation of new high-k candidate materials.