The emergence of hybrid metal halides (HMH) materials, such as the archetypal CH3NH3PbBr3, provides an appealing material platform for solution-processed spintronic applications due to properties such as unprecedented large Rashba spin-splitting states and highly efficient spin-to-charge (StC) conversion efficiencies. Here we report the first study of StC conversion and spin relaxation time in MAPbBr3 single crystals at room temperature using a spin pumping approach. Microwave frequency and power dependence of StC responses are both consistent with the spin pumping model, from which an inverse Rashba–Edelstein effect coherence length of up to ∼30 picometer is obtained, highlighting a good StC conversion efficiency. The magnetic field angular dependence of StC is investigated and can be well-explained by the spin precession model under oblique magnetic field. A long spin relaxation time of up to ∼190 picoseconds is obtained, which can be attributed to the surface Rashba state formed at the MAPbBr3 interface. Our oblique Hanle effect by FMR-driven spin pumping technique provides a reliable and sensitive tool for measuring the spin relaxation time in various solution processed HMH single crystals.