The morphology of nanocrystals is crucial in modulating their properties including optical, chemical and catalytic ones. For the intensively studied sheet-like structures, it is also important to engineer their detailed nanostructures on sheet surfaces. In this work, micron-sized bismuth oxychloride (BiOCl) thin square sheets in tetragonal matlockite-like phase and the corner-truncated ones were successfully synthesized by using a simple wet-chemical method. These square sheets could be partially etched, forming surface cracks with the size and density easily tuned. Two different types of cracks were observed on the surfaces of the corner un-truncated and truncated BiOCl square sheets. Surprisingly, radial cracks formed on the corner-truncated BiOCl sheets, which is attributed to the existence of physical stress during the etching and is highly related to the original nanostructure of the BiOCl sheets. This work provides a wet-chemical method for engineering surface cracks, especially radial cracks, on the surfaces of BiOCl nanosheets, which may be expanded to surface engineering of other nanosheets and will show a great potential in various fields. Nanocrystals, especially semiconductor ones, usually possess unique chemical, electrical, optical and magnetic properties compared to their bulk counterparts. [1][2][3][4][5][6] These properties are highly dependent on the chemical composition, size, shape and surface state of the nanocrystals. [3,[7][8][9][10][11] Therefore, controlled synthesis of nanocrystals is becoming a hot topic in many fields, and lots of efforts have been made to precisely control the morphology and surface state of the nanocrystals. [9,[12][13][14][15][16][17] Among various shaped nanocrystals, the sheet-like ones show promising properties and applications due to their structural simplicity, large surface area, easy charge separation, etc. [18][19][20][21] Sheet-like [a] R.