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The decay B-c(+) -> psi(2S)pi(+) with psi(2S) -> mu(+)mu(-) is observed with a significance of 5.2 sigma using pp collision data corresponding to an integrated luminosity of 1.0 fb(-1) collected by the LHCb experiment. The branching fraction of B-c(+) -> psi(2S)pi(+) decays relative to that of the B-c(+) -> J/psi pi(+) mode is measured to be B(B-c(+) -> psi(2S)pi(+))/B(B-c(+) -> J/psi pi(+)) = 0.250 +/- 0.068(stat) +/- 0.014(syst) +/- 0.006(B). The last term is the uncertainty on the ratio B(psi(2S) -> mu(+)mu(-))/B(J/psi -> mu(+)mu(-)). DOI: 10.1103/PhysRevD.87.071103