Grumpy Cropsies are the dirty and angry-looking ones, covered in purple slime. Cropsies become grumpy if they land on the purple slime that appears in some levels.
Why do Cropsies turn grumpy?
If you make a match that includes a grumpy Cropsie, the whole match will turn grumpy and they won't count toward your target goal. So be careful!
How can I clean up Grumpy Cropsies?
You can clean up Grumpy Cropsies by moving them to clean green grass.

Image shows a 'Grumpy' apple converted into a clean Cropsie by moving to the grass.
Pro tip: Depending on the level you might be able to return the grumpy Cropsies back to normal with grass created using seeds and water droplets. The Clean-Up Grumpy Cropsies booster will also do the trick.
Turn those frowns upside down!