Cellulose insulation polymer (paper/pressboard) has been widely used in high voltage direct current (HVDC) transformers. One of the most challenging issues in the insulation material used for HVDC equipment is the space charge accumulation. Effective ways to suppress the space charge injection/accumulation in insulation material is currently a popular research topic. In this study, an aluminium oxide functional film was deposited on a cellulose insulation pressboard surface using reactive radio frequency (RF) magnetron sputtering. The sputtered thin film was characterized by the scanning electron microscopy/energy dispersive spectrometer (SEM/EDS), X-ray photoelectron spectroscopy (XPS), and X-ray diffraction (XRD). The influence of the deposited functional film on the dielectric properties and the space charge injection/accumulation behaviour was investigated. A preliminary exploration of the space charge suppression effect is discussed. SEM/EDS, XPS, and XRD results show that the nano-structured Al 2 O 3 film with amorphous phase was successfully fabricated onto the fibre surface. The cellulose insulation pressboard surface sputtered by Al 2 O 3 film has lower permittivity, conductivity, and dissipation factor values in the lower frequency (<10 3 Hz) region. The oil-impregnated sputtered pressboard presents an apparent space-charge suppression effect. Compared with the pressboard sputtered with Al 2 O 3 film for 90 min, the pressboard sputtered with Al 2 O 3 film for 60 min had a better space charge suppression effect. Ultra-small Al 2 O 3 particles (<10 nm) grew on the surface of the larger nanoparticles. The nano-structured Al 2 O 3 film sputtered on the fibre surface could act as a functional barrier layer for suppression of the charge injection and accumulation. This study offers a new perspective in favour of the application of insulation pressboard with a nano-structured function surface against space charge injection/accumulation in HVDC equipment.