We showcase the use of high-resolution ion imaging with complementary state-resolved and "universal" vacuum ultraviolet probes to address a broad range of fundamental problems in chemical reaction dynamics. Examples from our recent work include applications in state-correlated unimolecular reactions, ion pair dissociation dynamics and spectroscopy, crossed-beam reactive scattering, and atomic angular momentum polarization in photodissociation. These studies are all directed to achieving a detailed understanding of atomic and molecular interactions, with particular emphasis on reaction mechanisms outside the scope of transition state theory; on spectroscopy and dynamics of highly excited, transient species; on nonadiabatic reaction mechanisms; and on chemical dynamics in polyatomic systems.