This work is devoted to the development of nanosphere lithography (NSL) technology, which is a low-cost and efficient method to form nanostructures for nanoelectronics, as well as optoelectronic, plasmonic and photovoltaic applications. Creating a nanosphere mask by spin-coating is a promising, but not sufficiently studied method, requiring a large experimental base for different sizes of nanospheres. So, in this work, we investigated the influence of the technological parameters of NSL by spin-coating on the substrate coverage area by a monolayer of nanospheres with a diameter of 300 nm. It was found that the coverage area increases with decreasing spin speed and time, isopropyl and propylene glycol content, and with increasing the content of nanospheres in solution. Moreover, the process of controllably reducing the size of nanospheres in inductively coupled oxygen plasma was studied in detail. It was determined that increasing the oxygen flow rate from 9 to 15 sccm does not change the polystyrene etching rate, whereas changing the high-frequency power from 250 to 500 W increases the etching rate and allows us to control the decreasing diameter with high accuracy. Based on the experimental data, the optimal technological parameters of NSL were selected and the nanosphere mask on Si substrate was created with coverage area of 97.8% and process reproducibility of 98.6%. Subsequently reducing the nanosphere diameter lets us obtain nanoneedles of various sizes, which can be used in field emission cathodes. In this work, the reduction of nanosphere size, silicon etching, and removal of polystyrene residues occurred in unified continuous process of plasma etching without sample unloading to atmosphere.