Here, we report an explorative study of an attempt to fabricate ultrathin aluminum oxide films on n-InP substrates by radio-frequency (RF) magnetron sputtering as a candidate for insulating layers in semiconductor lasers for optical communication. Film thickness and morphology were monitored to study the film growth and to explore the minimum thickness of a continuous film that RF magnetron sputtering could achieve. Originating from the weak wettability between the n-InP substrate and the Al2O3 film, Al2O3 films firstly grew in an island pattern which then turned into a layer-by-layer pattern when those islands became connected and continuous. Uniform and compact Al2O3 films were obtained when the film thickness reached 40 nm. The average transmittance, optical band gap, and optical absorption coefficient at a wavelength of 1550 nm of this Al2O3 film were about 80%, 3.72 eV, and 3.0 × 104 cm−1, respectively. At a frequency of 1 MHz, the permittivity, dielectric loss, and electrical resistivity were 8.96, 0.31, and 5 × 1010 Ω·cm, respectively. This work provides valuable references for the application of Al2O3 ultrathin films as insulating layers in micro-and opto-electronics.