Tw o-dimensional (2D) photocatalysts are highly attractive for their great potential in environmental remediation and energy conversion. Herein, we report anovel layered zinc silicate (LZS) photocatalyst synthesized by aliquid-phase epitaxial growth route using silica derived from vermiculite, al ayered silicate claym ineral, as both the lattice-matched substrate and Si source.The epitaxial growth of LZS is limited in the 2D directions,t hus generating the vermiculite-type crystal structure and ultrathin nanosheet morphology with thicknesses of 8-15 nm and al ateral sizeo fa bout 200 nm. Experimental observations and DFT calculations indicated that LZS has asuperior band alignment for the degradation of organic pollutants and reduction of CO 2 to CO.T he material exhibited efficient photocatalytic performance for 4-chlorophenol (4-CP) degradation and CO 2 conversion into CO and is the first example of ac laylike 2D photocatalyst with strong photooxidation and photoreduction capabilities.Supportinginformation and the ORCID identification number(s) for the author(s) of this article can be found under: https://doi.