Optical diffusion is an essential process used to manage photons in a wide range of photoelectric systems. This work proposes an approach to fabricate novel optical diffusers by a plasma-processing technique, using fiberform nanostructures formed by helium plasma irradiation and subsequent annealing. After an annealing procedure in the air for oxidation, the optical properties and the light-diffusing abilities of these nanostructured thin films were studied. In addition to the morphology analysis and total transmittance measurement, the diffusion efficiency of the optical diffusers was analyzed using a transmitted scatter distribution function (TDF). It was revealed that the diffusion efficiency of a device with an irradiation time of 30 minutes could reach 97%. The results demonstrate the potential of these nanostructured optical diffusers for various photoelectric applications.