High quality La2/3Ca1/3MnO4(LCMO) thin films have been deposited on silicon-on-insulator (SOI) substrates only buffered by yt tria-stabilized zirconia (YSZ) by using the pulsed laser deposition (PLD) technique. The results obtained from X-ray diffraction (XRD), reflection high energy electron diffraction (RHEED), scanning electron microscopy (SEM) and magnetization investigations indicate that the LCMO films are highly oriented both in-plane and out-of-plane. The Curie temperature Tc is close to 260 K and the insulator–metal (I–M) transition appears around 220 K. The conducting mechanism at low temperatures is dominated by the electron–magnon scattering. A tensile stress from the film–substrate lattice mismatch results in magnetic ‘easy axes’ in the film plane and the magnetic anisotropy energy increases with cooling. A maximum magnetoresistance (MR) is observed near 190 K, with the external magnetic field either parallel or vertical to the LCMO film plane. Moreover, the large intrinsic high-field magnetoresistance (HFMR) and the very small extrinsic low-field magnetoresistance (LFMR) again reveal that the LCMO films on SOI substrates are highly oriented thin films of good crystallinity.