We demonstrate spin squeezing and entanglement in a large-spin system via quantum non-demolition measurement. We make non-destructive, projection-noise-limited collective spin measurements on an ensemble of up to in 8.4 × 105 laser-cooled 87Rb atoms in the f = 1 hyperfine ground state. A dynamically-decoupled probing scheme [Phys. Rev. Lett. 105, 093602 (2010)] prevents probe-induced decoherence. Repeated measurements show correlations beyond the standard quantum limit, indicating generation of a spin-squeezed state with up to −3.6 dB of noise reduction and −2.6 dB of metrologically-relevant squeezing.