Other than removed selected really large pieces, such as entire derelict spacecraft, in crowded orbits like GEO where the likelihood of hitting something else is high.
Also, depending on the orbit considered, the debris generated by the harpoon may be less harmful: they have typically a high surface area/weight ratio so they will deorbit fast if the altitude is low enough, like for this mission.
Smaller things are more likely to burn up on reentry, whereas bigger things can partially survive.
Atmospheric drag can also vary based on size and density of debris. IIRC smaller things will reenter more quickly. Which is nice, except smaller debris is harder to track (imagine looking for a fleck of paint that's 500 miles away).
However things are a little different in GEO. The good news is that orbital velocities are lower, so if you hit something it'll be less catastrophic than if you hit it at the same angle in LEO. But tracking things is much harder. In LEO you can follow the wrench that some astronaut dropped 10 years ago. But in GEO there's almost no chance. And there's much less atmospheric drag, so junk can stay up there for hundreds of years.
For killing a spacecraft? Small debris. For creating more debris? Big debris.
In addition, small space debris could conceivably be cleaned up with lasers from the ground. That's not so feasible for bigger stuff.