Your tiles don't fit the background grid. For your tall tiles, the bottom sprite boundary aligns with the low edge, but the top sprite boundary aligns with the high edge. On the right, I've marked the tile size you provided in blue, and the actual tile size in red.
Additionally, the hexagons on the bottom have a different shape than the hexagons on the top: on the left, I marked the bottom hexagon outline in blue and overlaid the top outline in red. They'll never fit together properly.
If you want to create proper hex grids, you'll need a fixed template shape that serves as the base of your hexagonal prisms, not the entire outline. You can make the actual tiles as tall as you want, as long as the base is always in the same shape and at the same position. Of course the bottom slope needs to be the same as the top slope too.
If you want your hexagons to be regular hexagons, then the vertical ratios of the template need to be 1:2:1 as depicted here:
The ratio of height to width is left up to you, it will correspond to a different apparent view angle.