This Frontier presents the recent developments and applications of two-dimensional (2D) amorphous transition metal oxides (TMOs) obtained by using supercritical CO2. CO2 molecules can affect the crystal transformation of layered materials and allow diffusive atomic disordering during the exfoliation process. If amorphous structures are introduced into TMOs, the strong localization tail states that exist in the band gap of TMOs can effectively promote chemical reactions. We also discuss the future challenges to be overcome for this class of supercritical CO2 and 2D amorphous materials.