Monolayer and bilayer colloidal-crystal films are used as physical mask in nanosphere lithography (NSL). So far, spin-coating experiments have mainly been designed to form nanosphere monolayer with one given size or obtain small areas of polystyrene (PS) nanosphere monolayer which limited the application of these films used as physical masks. The development of NSL required more study focused on the preparation of colloidal-crystal films with large-scale, high ordering degree and nanospheres of different diameters. In this study, PS nanospheres were self-assembled to form monolayer and bilayer colloidal-crystal films by employing spin-coating technology. Based on our experiments, we have built an experiment system of PS nanospheres of certain size ranging from 200 nm to 1300 nm. To give an instance, we have chosen PS nanospheres of four diameters (223 nm, 347 nm, 509 nm, 1300 nm) to fabricate colloidal-crystal films by adjusting the spin speed and acceleration, and we have investigated the relationship between the monolayer coverage areas and spin parameters by designing different spin speed and acceleration for 509 nm nanosphere. Results revealed that monolayer and bilayer films of PS nanospheres with four different diameters were prepared successfully and the single structure where PS nanospheres were in hexagonal close-packed (HCP) order dominated the surface morphologies of both monolayer and bilayer colloidal-crystal films. For 509 nm PS nanosphere, as the spin speed and acceleration increasing, the monolayer coverage areas increase firstly then decrease and at spin speed 1750 rpm and acceleration 600 rpm/s, the areas reaches the biggest. (c) 2013 Published by Elsevier B.V.