We are able to grow high quality La0.67Sr0.33MnO3(LSMO) colossal magnetoresistive (CMR) thin films on Y‐stabilized zirconia (YSZ) buffered (100) Si substrates using a Bi4Ti3O12 texturing and lattice matching layer. The CMR films have very high structural perfection and show excellent transport and ferromagnetic properties, including the almost full saturation magnetization values and narrow ferromagnetic resonance peaks (15 Oe at 290 K). The lattice matching template/buffer layer approach is suitable for the high quality CMR films on Si. A close correlation between the magnetic hysteresis loop and the field dependence of MR is observed at lower temperatures.