I believe that a unit that enters the space/atmosphere interface while out of control is auto-dead, so immediately before reentry seems the most efficient time to crack the egg. Downside is that you have to hit it with big stuff that can threshold it so you can force control rolls. Regular hits don't force the lawn-dart until you're in atmosphere. So AC/20s, Heavy Large Lasers, Anti-Ship Missiles...if you've actually got a DropShip of your own, this is the time to use it. I forget which hit chart had the best odds of Control Roll crits, but that's what you want. Pepper the ship in lots of hits just big enough to threshold...in an Overlord that means 2-points Capital up the tailpipe, and 3 Capital anywhere else.
If it makes it through reentry, then don't worry about thresholding, unless playing with the rule where only threshold-capable hits count toward lawn-dart checks. At this point you want to keep harassing that Overlord all the way down. Keep hitting it with something, anything every turn, keep going for that lawn-dart. Heck, Overlords aren't that tough, if you just keep up a sustained barrage there's a very real chance you'll crack it the hard way before it can land.
If you've still got stuff that can threshold, go for side hits(you'll likely be forced into this anyway by dead zones), and hope for Door crits. You break a door, that's one less the ship can use to drop mechs before the egg cracks, and will also slow down offloading when on the ground, giving you more time to kill the ship while there's still mechs inside.
Moral of the story: To quote Jellico, just shoot the damned thing. Lots.