An easy way to increase the eccentric (negative) loading is to do the concentric or lifting part of the rep with both legs, then the lowering part with one leg. After you hit failure with the single-leg eccentrics, continue the set by using both legs and a controlled negative.
Alternate legs on each rep. Make sure to do the eccentric portion in a controlled fashion to take advantage of the overloading effect. Don't just let your leg freefall when lowering the weight. Do 4 sets of 8 reps.
It's a fact: the exercises that make you hate life the most also tend to deliver the best results. If you're in serious need of a hamstring overhaul, then this article is a great (although painful) place to start.