Microchannel plate (MCP) as a key part is a kind of electron multiplied device applied in many scientific fields. Oxide thin films such as zinc oxide doped with aluminum oxide (ZnO:Al2O3) as conductive layer and pure aluminum oxide (Al2O3) as secondary electron emission (SEE) layer were prepared in the pores of MCP via atomic layer deposition (ALD) which is a method that can precisely control thin film thickness on a substrate with a high aspect ratio structure. In this paper, nano-oxide thin films ZnO:Al2O3 and Al2O3 were prepared onto varied kinds of substrates by ALD technique, and the morphology, element distribution, structure, and surface chemical states of samples were systematically investigated by scanning electron microscopy (SEM), energy-dispersive X-ray spectroscopy (EDS), X-ray diffraction (XRD), and X-ray photoemission spectroscopy (XPS), respectively. Finally, electrical properties of an MCP device as a function of nano-oxide thin film thickness were firstly studied, and the electrical measurement results showed that the average gain of MCP was greater than 2,000 at DC 800 V with nano-oxide thin film thickness approximately 122 nm. During electrical measurement, current jitter was observed, and possible reasons were preliminarily proposed to explain the observed experimental phenomenon.