The invention provides a laminated dielectric layer for semiconductor devices formed by a combination of ZrO₂ and a lanthanide oxide on a semiconductor substrate and methods of making the same. In certain methods, the ZrO₂ is deposited by multiple cycles of reaction sequence atomic layer deposition (RS-ALD) that includes depositing a ZrI₄ precursor onto the surface of the substrate in a first pulse followed by exposure to H₂O/H₂O₂ in a second pulse, thereby forming a thin ZrO₂ layer on the surface. After depositing the ZrO₂ layer, the lanthanide oxide layer is deposited by electron beam evaporation. The composite laminate zirconium oxide/lanthanide oxide dielectric layer has a relatively high dielectric constant and can be formed in layers of nanometer dimensions. It is useful for a variety of semiconductor applications, particularly for DRAM gate dielectric layers and DRAM capacitors.