We have investigated the influence of substitution of Sr for Ba on the structure, charge distribution, and T c in the YBa 2 Cu 4 O 8 ͑Y124͒ compound. Bond valence sum and nuclear quadrupole resonance investigations show that the substitution of Sr causes a redistribution of charge in the structure. The number of holes located in plane copper ͑Cu2͒ and apical oxygen ͑O1͒ increases, hence the number of holes in chain copper ͑Cu1͒ and plane oxygen ͑O2 and O3͒ decreases. A redistribution of holes from Cu1 to O1 and from O2 and O3 to Cu2 takes place. The literature data for Y123 and the hydrostatic pressure effect on both Y124 and Y123 compounds show that oxygen doping in Y123 and the pressure effect in Y124 increase the hole number equally on copper and oxygen. Therefore, although the number of holes on copper Cu2 in the CuO 2 planes increases with Sr doping in both Y124 and Y123, T c does not rise as much as expected from the amount of charge transferred to Cu2, because of their distribution in the CuO 2 planes.