Reduce your game window size to match native PS2 resolution. These games were made before HD monitors, so without some serious filters they aren't going to look Perfect.

The first image does look like in-game fog effects making it look somewhat blurry, where the second image looks very pixelated as you would expect from a game made for SD television. I also see that the second image says 66% speed on the title screen, which leads me to believe you aren't going to get the look and performance you want without reducing the window size.