Ultrafast atomic and molecular photoexcitation and relaxation pathways evolve on few-femtosecond timescales and play a defining role in photochemistry or material processing. The dynamics are commonly observed using pump-probe schemes utilizing few-fs or attosecond pulses. The presentation will overview the realization of different schemes used for the investigation of ultrafast atomic and molecular dynamics in gas-phase targets. First, a XUV-pump / XUV-probe setup will be presented, where nonlinear excitation dynamics in the XUV spectral region are the ultrafast processes of interest. Second, a scheme utilizing µJ-level few-fs VUV pulses for the investigation of early-time ultrafast molecular relaxation dynamics is introduced and discussed. The final topic will cover a combination of both presented approaches aiming to investigate ultrafast molecular dynamics with a VUV-pump / XUV-probe scheme.