MRSF-TDDFT has several advantages over SF-TDDFT, the most significant being that spin contamination is drastically reduced, simplifying the identification of relevant states. This is important for excited-state ge- ometry optimization, reaction-path following, and TSH simulations. (Notably, the analytic gradient has been formulated for MRSF-TDDFT, along with approximate nonadiabatic couplings, whereas no analytic gradient for SA-SF-TDDFT is yet available.) MECP geometries are found to be in good agreement with multireference benchmarks but also in good agreement with the simple SF-TDDFT method, whereas vertical excitation energies are comparable in accuracy or slightly better with MRSF. Both of these comparisons are based on the BH&HLYP functional, which is also used in nearly all of the SF-TDDFT results quoted in this chapter. Interestingly, when the fraction of exact exchange (C HFX ) is optimized in order to minimize errors in vertical excitation energies of polyenes, the MRSF-TDDFT approach lands on C HFX = 0.5 as the optimal value, corresponding precisely to the BH&HLYP functional. The same optimization procedure applied to LR-TDDFT lands on C HFX = 0.2 as the optimal value, corresponding to B3LYP. This observation further corroborates the idea that 50% HFX is close to optimal for collinear spin-flip methods.