A substrate processing method is provided, which includes: a substrate holding step of causing a substrate holding unit to hold a substrate; an ozone-containing hydrofluoric acid solution supplying step of supplying an ozone-containing hydrofluoric acid solution containing ozone dissolved therein a hydrofluoric acid solution to one major surface of the substrate held by the substrate holding unit; a brush-cleaning step of cleaning the one major surface of the substrate by bringing a cleaning brush into contact with the one major surface of the substrate after the ozone-containing hydrofluoric acid solution supplying step; and an ozone water supplying step of supplying ozone water to the one major surface of the substrate before start of the brush-cleaning step after the ozone-containing hydrofluoric acid solution supplying step or in the brush-cleaning step.