A substrate processing method is provided, which includes: an ozone-containing hydrofluoric acid solution spouting step of spouting an ozone-containing hydrofluoric acid solution containing ozone dissolved therein from a nozzle toward one major surface of a substrate held by a substrate holding unit; and a brush-cleaning step of cleaning the one major surface of the substrate by bringing a cleaning brush into abutment against the one major surface of the substrate, the brush-cleaning step being performed after the ozone-containing hydrofluoric acid solution spouting step or in parallel with the ozone-containing hydrofluoric acid solution spouting step.