The suppressed decay Λb0 → pπ−μ+μ−, excluding the J/ψ and ψ(2S) → μ+μ− resonances, is observed for the first time with a significance of 5.5 standard deviations. The analysis is performed with proton-proton collision data corresponding to an integrated luminosity of 3 fb−1 collected with the LHCb experiment. The Λb0 → pπ−μ+μ− branching fraction is measured relative to the Λb0 → J/ψ(→μ+μ−)pπ− branching fraction giving
B(Λ0b→pπ−μ+μ−)B(Λ0b→J/ψ(→μ+μ−)pπ−)=0.044±0.012±0.007,
where the first uncertainty is statistical and the second is systematic. This is the first observation of a b → d transition in a baryonic decay.