A pixel arrangement structure, a display substrate, a display device, and a mask plate set are provided. In the pixel arrangement structure, a first virtual rectangle includes one first color sub-pixel block, one second color sub-pixel block, and one third color sub-pixel block, the first virtual rectangle includes a first edge and a second edge; a distance between the second color sub-pixel block and the first edge and a distance between the third color sub-pixel block and the first edge are both smaller than a distance between the first color sub-pixel block and the first edge; and a center of the first color sub-pixel block is located on the perpendicular bisector of the first edge and a distance between the center of the first color sub-pixel block and the first edge is approximately ½ to ¾ of a length of the second edge.