We use optical transient-grating spectroscopy to measure spin diffusion of optically oriented electrons in bulk, semi-insulating GaAs(100). Trapping and recombination do not quickly deplete the photoexcited population. The spin diffusion coefficient of 88 ± 12 cm 2 /s is roughly constant at temperatures from 15 K to 150 K, and the spin diffusion length is at least 450 nm. We show that it is possible to use spin diffusion to estimate the electron diffusion coefficient. Due to electron-electron interactions, the electron diffusion is 1.4 times larger than the spin diffusion. The burgeoning field of semiconductor spintronics relies on moving spin-polarized electrons through distances comparable to the dimensions of an electronic device. The importance of spin transport has led to several studies of spin diffusion in GaAs quantum wells. Spin transport in quantum wells can differ markedly from the bulk material, due to to different scattering rates and especially to the different spin-orbit coupling 1 . Nonetheless, there have been relatively few measurements 2-4 of spin diffusion in bulk GaAs. In n-doped samples with n = 1 × 10 16 and 2 × 10 16 cm −3 , the spin diffusion coefficient D s ranged from 10 to 200 cm 2 /s. Spin diffusion in semi-insulating GaAs (SI-GaAs) has not been reported. SI-GaAs has been proposed as a platform for nuclear spintronics 5 due to its low carrier density. Moreover, Kikkawa et al. showed that electrons could be optically oriented in SI-GaAs and would subsequently diffuse into an adjacent ZnSe film, maintaining their spin polarization 6 . Since SI-GaAs is a ubiquitous substrate material for thin film growth and for spintronic devices, such spin diffusion is of practical consequence, whether intentional or not. In this work, we find that SI-GaAs has a large, temperature-independent spin diffusion coefficient.We measured spin diffusion with an ultrafast transient spin grating 7 , which measures the decay rate γ s of a spin-density wave (the "grating") with wavelength Λ and wavevector q = 2π/Λ. The grating amplitude decays-through spin relaxation, electron-hole recombination, and diffusion-at a rate of Here, D s is the spin diffusion coefficient, and τ 0 is the lifetime for trapping, recombination, and spin relaxation. Measurement at several q determines D s . We measure in a reflection geometry, and improve the detection efficiency by heterodyne detection 8 . Noise is further suppressed by 95 Hz modulation of the grating phase and lock-in detection 9 . The SI-GaAs sample was grown by Wafer Technology. It was undoped, oriented (100), had room temperature resistivity ρ ≥ 107 Ω-cm and Hall mobility µ H ≥ 5000 cm 2 /V-s. The pump and probe pulses came from a mode-locked Ti:Sapphire laser with wavelength near 800 nm and repetition rate of 80 MHz. The two pump pulses were focused to a spot of 65 µm diameter with total fluence 3.0 µJ/cm 2 except as indicated; probe pulses were always a factor of 2.5 weaker. Assuming one photoexcited electron per absorbed photon in a 1 µm absorption length 10 , we p...