  We report on a novel method for photo-association of strongly polar trilobite
Rydberg molecules. This exotic ultralong-range dimer, consisting of a
ground-state atom bound to the Rydberg electron via electron-neutral
scattering, inherits its polar character from the admixture of high angular
momentum electronic orbitals. The absence of low-$L$ character hinders standard
photo-association techniques. Here, we show that for suitable principal quantum
numbers resonant coupling of the orbital motion with the nuclear spin of the
perturber, mediated by electron-neutral scattering, hybridizes the trilobite
molecular potential with the more conventional ${\rm{S}}$-type molecular state.
This provides a general path to associate trilobite molecules with large
electric dipole moments, as demonstrated via high-resolution spectroscopy. We
find a dipole moment of 135(45) D for the trilobite state. Our results are
compared to theoretical predictions based on a Fermi-model.
