A methodology is described for the experimental and theoretical study of surface roughness (SR) and line-edge roughness (LER) and their relation for solution and plasma developed resist schemes. Experimental results for a negative-tone nonchemically amplified siloxane bilayer resist scheme are shown. In addition, a molecular-type simulation of SR and LER is presented. The simulator can follow the appearance of SR and LER after each process step and predict the roughness dependence on material properties and process conditions. The simulation results are compared with SR experimental data for a negative-tone chemically amplified epoxy resist.