A pixel arrangement structure, a display substrate, and a display device. The pixel arrangement structure comprises pixel groups (10) extending in a first direction and arranged in a second direction, and each pixel group (10) comprises a first sub-pixel row (100), a second sub-pixel row (200), and a third sub-pixel row (300). The first sub-pixel row (100) comprises a plurality of first sub-pixels (110), the second sub-pixel row (200) comprises a plurality of second sub-pixel pairs (210), and the third sub-pixel row (300) comprises a plurality of third sub-pixels (310). The pitches of the plurality of first sub-pixels (110), the plurality of second sub-pixel pairs (210), and the plurality of third sub-pixels (310) in the first direction are same. In each pixel group (10), a line connecting the centers of a first sub-pixel (110) and a third sub-pixel (310) adjacent to each other are substantially parallel to the second direction, and the first sub-pixel row (100) and the second sub-pixel row (200) are shifted by one half of the pitch in the first direction. The orthographic projections of a second sub-pixel pair (210) and a first sub-pixel (110) adjacent to each other on a straight line extending in the first direction are overlapped, and the first sub-pixel rows (100) in the two adjacent pixel groups (10) are shifted by one-half of the pitch in the first direction. The pixel arrangement structure reduces the grainy sensation of the second sub-pixel pairs during display.