The excited-state carrier dynamics of lead halide perovskites play a critical role in their photoelectric properties, and are greatly affected by lattice structural changes. In this work, the carrier dynamics of all-inorganic CsPbBr3 peroveskite, as a function of pressure, are investigated using in situ high-pressure femtosecond transient absorption spectroscopic experiments. Compression is found to drive crystal structural evolution, thereby markedly changing the behavior of charge carriers in CsPbBr3. Before the phase transition, simultaneous prolonging of the carrier relaxation and Auger recombination is achieved alongside a narrowing in the bandgap. The results favor improved efficiency and photovoltaic performance.