Also try using mechanically interlocking features. Since this is highly recommended for injection moulding in overmoulding, according to the manuals, I think it also applies for 3D-printing. At least, it shouldn't hurt.
Think of a dovetail system, or hooks, or chains that interlock. Think of these concepts, but then all melted and squeezed into one solid block.
Have a look at how it is done in tooth brushes: most of them also have overmoulding with interlocking features.
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Dim3nsioneer 558
If you can, change one of the materials. The second table on this page shows you compatible materials. As you can see, PLA and TPU is not a supported combination.
ABS/TPU or PC/TPU should work quite well.
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