High-resolution atomic pair distribution functions have been obtained using neutron powder diffraction data from La2-xSrxCuO4 over the range of doping 0<or=x<or=0.30 at 10 K. Despite the average structure getting less orthorhombic, we see a broadening of the in-plane Cu-O bond distribution as a function of doping up to optimal doping. Thereafter the peak abruptly sharpens. The peak broadening can be well explained by a local microscopic coexistence of doped and undoped material. This suggests a crossover from a charge inhomogeneous state at and below optimal doping to a homogeneous charge state above optimal doping.