Herein, interfacial reconstruction in a series of La0.7Sr0.3MnO3 (LSMO) films grown on a (001) oriented LaAlO3 (LAO) substrate using the pulsed plasma sputtering technique is demonstrated. X-ray diffraction studies suggested that the LSMO film on LAO was stabilized in a tetragonal structure, which was relaxed in-plane and strained along the out-of-plane direction. The interfacial reconstruction of the LSMO-LAO interface due to the reorientation of the Mn ion spin induced spin-glass behavior due to the presence of non-collinear Mn ion spins. Consequently, the interface effect was observed on the Curie temperature, temperature-dependent resistivity, metal-to-semiconductor transition temperature, and magnetoresistance (MR). At a magnetic field of 7 T, MR decreased from 99.8% to 7.69% as the LSMO film thickness increased from 200 Å to 500 Å. A unique characteristic of the LSMO films is the large low-field MR after a decrease in the field from the maximum field. The observed temperature-dependent magnetization and low-temperature resistivity upturn of the LSMO films grown on LAO provide direct evidence that the low-field MR is due to the non-collinear interfacial spins of Mn. The present work demonstrates the great potential of interface and large low-field MR, which might advance the fundamental applications of orbital physics and spintronics. © The Royal Society of Chemistry.